• <tr id="yyy80"></tr>
  • <sup id="yyy80"></sup>
  • <tfoot id="yyy80"><noscript id="yyy80"></noscript></tfoot>
  • 99热精品在线国产_美女午夜性视频免费_国产精品国产高清国产av_av欧美777_自拍偷自拍亚洲精品老妇_亚洲熟女精品中文字幕_www日本黄色视频网_国产精品野战在线观看 ?

    Present and Future of Phase?Selectively Disordered Blue TiO2 for Energy and Society Sustainability

    2021-03-08 09:30:06YongguangLuoHyoyoungLee
    Nano-Micro Letters 2021年3期
    關(guān)鍵詞:心弦一串串連線

    Yongguang Luo, Hyoyoung Lee,3,4

    ABSTRACT Titanium dioxide (TiO2) has garnered attention for its promising photocatalytic activity, energy storage capability, low cost, high chemical stability, and nontoxicity. However, conventional TiO2 has low energy harvesting efficiency and charge separation ability, though the recently developed black TiO2 formed under high tem?perature or pressure has achieved elevated performance. The phase?selectively ordered/disordered blue TiO2 (BTO), which has visible?light absorption and efficient exciton disassociation, can be formed under normal pres?sure and temperature (NPT) conditions. This perspective article first discusses TiO2 materials development mile?

    KEYWORDS Blue TiO2 (BTO); Phase?selective disordering; Visible?light?driven photocatalyst; Charge separation; Energy and society sustainability

    1 Introduction

    Modern society has achieved great science and technol?ogy explosion to date but faces severe energy demands and environmental concerns to realize sustainable development. One crucial issue in the twenty?first century is finding ways to convert and store renewable energy efficaciously while tackling climate change and environmental pollution caused by unsustainable human activity. In that context, titanium dioxide (TiO2) has received a lot of attention for its photo?catalytic activity, energy storage capability, low cost, high chemical stability, and nontoxicity. The initial discovery of the photocatalytic potential of TiO2dates back to the end of the 1920s [1]. Researchers observed that aniline dyes faded and fabrics degraded in the presence of TiO2, oxygen gas (O2), and ultraviolet (UV) light. However, the academic community did not show strong scientific enthusiasm about the phenomenon at that time due to a lack of interest in renewable energy and environmental stewardship.

    That began to change after Fujishima and Honda reported the discovery of water photoelectrolysis into hydrogen (H2) by rutile TiO2under UV irradiation in 1969 [2]. The Honda-Fujishima water splitting finding was refined and called “natural photosynthesis” byNaturein 1972 [3]. Now, TiO2is one of the most promising photocatalyst materials. Its valence band (VB) and conduction band (CB) positions offer more diverse catalysis reaction potential than available with many other transition metal oxides and dichalcogenides [4]. Furthermore, the heterogeneous photocatalysis of TiO2enables smoother industrial recycling than is available for homogeneous photocatalysts.

    TiO2has three main polymorphs, anatase, rutile, and brookite. The anatase and rutile phases of TiO2are the most frequently studied and synthesized in laboratories and industry, whereas brookite, as a natural phase, is rarely investigated as a photocatalyst due to difficulties in synthe?sizing it [5]. The anatase phase is reported to have higher photocatalytic performance than the rutile phase because it has better bulk charge transportation and a smaller recom?bination portion of the exciton [6, 7]. After several decades of developments, various TiO2synthesis approaches have been established through gas?phase reactions, solution?based methods, and alcoholysis from titanium tetrachloride (TiCl4) [8], titanium oxysulfate (TiOSO4) [9], and Ti(OC4H9)4[10]. To date, one of the famous TiO2photocatalyst products is commercial Degussa P?25 (P25) (Degussa Co., Ltd), which has been frequently applied as a benchmark photocatalyst [11, 12]. P25 TiO2contains a unique hybrid of anatase and rutile phases in a roughly 3:1 ratio and exhibits good per?formance in many photocatalytic systems [13]. TiO2is also used in other industries: energy (energy production and stor?age), environment (degrading pollution in the air, wastewa?ter, and indoors), human health and food (antibacterial, anti?virus sterilization), cosmetics (sunscreen against UVA and UVB), and self?cleaning and antifogging products [14, 15]. The antivirus potential of TiO2will certainly draw atten?tion during the struggle with the COVID?19 coronavirus pandemic [16].

    TiO2still faces several hindrances to its photocatalytic performance. First, pristine TiO2can absorb sunlight only in the UV region (5%) due to its large electronic bandgaps (anatase, 3.2 eV; rutile 3.0 eV), which results in extremely low photocatalysis quantum efficiency that fails to meet the needs of industrial applications. Second, the separated charges (electrons and holes) formed after photoexcitation of a photocatalyst can recombine and disappear, giving sub?sequent photoluminescence. This exciton recombination process reduces the number of active electrons and holes on the photocatalyst surface, which is detrimental to any photocatalysis reaction. Therefore, research is needed to boost light absorption efficiency and block charge recom?bination to maintain a high exciton dissociation capability. Many attempts have been made to attain a broader range of light absorption by using non?metallic elements (C, N, and S) [17] and transition metal doping [18, 19] to tune the TiO2electronic structure. However, only a few researchers have tried to develop advanced TiO2by targeting both vis?ible?light absorption and high charge separation efficiency. Those efforts produced “Black TiO2” [20] and “Blue TiO2” [21] in 2011 and 2016, respectively. In addition, the phase?selectively disordered blue TiO2(BTO) offers high H2gen?eration performance through its three unique phase-interface configurations.

    Next, we summarize several historical milestones in the development of TiO2materials and then systematically illus?trate the development logic and discovery of BTO, includ?ing its mild synthesis conditions, robust reducing agent design, and phase?selective disordering. The phase selec?tivity of BTO results from its unique structure, which we disclose on the crystalline dimension level, and the reduction power of alkali metal amines. Its ordered?disordered phase junctions, type II band alignment structure, and a surface rich in hydroxyl groups explain the high exciton dissociation efficiency, visible?light absorption, and superior photoca?talysis of BTO. Particularly, we further present the explora?tory attempts of BTO in various energy and environmen?tal aspects. Finally, we suggest future research avenues to explore the potential of BTO further.

    2 Milestones in TiO2 and the Development of BTO

    The research community has long worked to exploit the energy efficiency and activity of TiO2in versatile applica?tions. Events of considerable significance in the recent his?tory of TiO2development are shown in Fig. 1a. The first fundamental finding in TiO2photocatalysis for energy con?version was a report of water electrochemical photolysis which generates the absolute clean energy gas, H2, using a rutile TiO2semiconductor electrode in 1972 by Fujishima and Honda et al. However, the applied rutile TiO2has lower charge transportability than anatase TiO2, even though it has better light absorption efficiency to generate more charges. The underlying reasons that anatase has better charge transportation than the rutile phase are the higher VB maximum energy level of the anatase phase (Fig. 1b) [7], its preferred crystalline surface orientation [22], and its longer exciton (electron and hole pair) lifetime [23]. To use the advantages of both the anatase and rutile phases, the commercially available phase?mixed P25 TiO2has been widely used as a standard photocatalyst. It has been proved a better activity than the single?phase TiO2since the 1990s [13, 24, 25]. Extending the TiO2light absorption range was the main challenge after the development of P25. In 2011, Xiaobo Chen et al. found that TiO2phase disorder engi?neering through hydrogenation enhanced its light absorp?tion capability into the visible and infrared ranges [20]. That hydrogenated black TiO2mostly answered concerns about the photocatalysis energy efficiency of TiO2. Moreo?ver, the photocatalytic activity of black TiO2is boosted by suppressing exciton recombination through the middle VB by means of localized holes generated in the disordered sur?face. During approximately four decades of research, TiO2material development has produced decent UV-visible?light absorption, acceptable photocatalytic activity, and reason?able charge generation. Nevertheless, TiO2still requires more development to be practical for energy production and photocatalysis applications. After thoroughly investigating the recent achievements in black TiO2material design, we found that most black TiO2synthesis approaches require high temperatures (400-900 °C) or a high H2atmospheric pressure (20-70 bar) [26]. Furthermore, the black TiO2core/shell structure produces a back reaction that diminishes its photocatalytic power because of its sole surface reaction interface. The issues that remain to be addressed since the development of black TiO2are developing an industrially suitable manufacturing process with mild conditions and further strengthening exciton dissociation and catalytic reac?tion efficiency.

    3 NPT Synthesis of BTO and Its Phase?selective Specialty

    The high?temperature and H2atmospheric pressure synthe?sis conditions of most black TiO2are energy?intensive and potentially explosive, an unfavorable manufacturing choice in both laboratories and industry. Therefore, it is essential to find a suitably, potent reducing agent or system. Birch reduction agents, an alkali metal in liquid ammonia, can reduce arenes into cyclohexadiene rather than cyclohexane [27]. Among the Birch reduction processes, the electride salts that form by mixing an alkali metal (M) and ammonia (NH3) as [M(NH3)x]+e?have strong reducing power. There?fore, we supposed that producing such vital electride salts as a reduction species would contribute to TiO2reduction. We found that a lithium ethylenediamine (Li?EDA) solu?tion reduced the rutile phase of P25 TiO2while keeping the anatase phase intact, which resulted in a unique blue TiO2product (BTO(I)) [21].

    The superior photocatalysis performance of BTO stimu?lated us to investigate the origin of its phase selectivity fur?ther. As shown in Fig. 2a, the free electron of M?EDA elec?trides can attack the firm Ti-O bond and produce a reduced Ti3+state. The evidence for Ti3+and oxygen vacancy (OV) were provided by X?ray photoelectron spectroscopy and electron paramagnetic resonance in our previous reports from 2015 to 2019, respectively. Besides, the reduced TiO2is generally presented in a disordered amorphous physical state with a black appearance. The blue color of BTO is caused by the coexistence of an ordered crystalline anatase (Ao) phase and a disordered amorphous rutile (Rd) phase. The successful reduction of TiO2by a Li?EDA solution in normal pressure and temperature (NPT) conditions indicates its mighty reducing power. It successfully replaced the high pressure and temperature hydrogenation reduction approach.

    Fig. 1 a Milestones in TiO2 material development and b the corresponding band structure of each typical TiO2 configuration [3, 20, 21, 25, 28, 32]. The TiO2 nanoparticles illustration figures in (a) are adapted with the permission from Ref. [28]. Copyright (2019) American Chemical Society

    After successfully preparing ordered anatase (Ao)/disor?dered rutile (Rd) TiO2from P25 with the Li?EDA solution under NPT conditions, we set out to design disordered anatase (Ad)/ordered rutile (Ro) TiO2from P25. With the curiosity of other alkali metal EDA reduction phenomena, we applied Na and K EDA solutions to reduce the P25. Interestingly, the Na/K?EDA solution selectively reduced the P25 TiO2reverse from the Li?EDA. Figure 2b shows that P25 TiO2turns to Rd/Ao(BTO(I)) through Li?EDA reduction and Ro/Ad(BTO(II)) through Na/K?EDA reduc?tion. Furthermore, the anatase and rutile phases TiO2were individually treated by Li?EDA and Na/K?EDA, respectively. The pure white rutile TiO2becomes black RdTiO2in a Li?EDA environment, and the anatase sin?gle?crystalline form becomes black or gray AdTiO2after the Na/K?EDA reduction. Based on that initial finding, which we were the first to report, the TiO2architecture can be widely enriched to extend its potential applications. Because of their blended ordered and disordered phase structure, BTO(I) and BTO(II) have high potential as pho?tocatalysts with effective heterojunctions and visible?light absorption. In addition, the M?EDA?reduced Rdand Adcan be used to anchor hybrid material systems and maintain a steady structure through covalent combinations.

    To investigate the best amines for dissolving alkali met?als and reducing TiO2, we selected various liquid amine derivatives, including monoamines with different alkyl chain lengths (Numb. 1-4 in Fig. 2c) and diamines with diverse alkyl chain lengths and positions (Numb. 5-8 in Fig. 2c). The various M?amine solutions produced diverse forms from the P25 that were colored from blue to gray. Among them, the shortest alkyl chain diamine solution, Na?EDA, exhibited the best reduction results, producing a deep blue color and entirely vanished anatase crystalline phase, as shown in the detailed XRD characterization in Ref. [28]. EDA’s effects result from its effective diamine structure and higher polar?ity than the long alkyl chain amines, which contribute to its high alkali metal solubility. This newly developed, powerful reducing system (M?EDA) can be readily extended to the reduction of other metal oxides or metal sulfides and defect design objectives.

    Next, we examined the crystallography of anatase and rutile TiO2at the atomic level to find the origins of the phase selectivity. Beginning with facet information about the rutile (110) and anatase (101) phases [28-30], we found the gap distance in the unit lattice to be around 2.96 ? × 2.96 ? for rutile (110) and 2.86 × 3.79 ?2for anatase (101), as shown in Fig. 2d. The diameters of Li, Na, and K atoms in the EDA environment are 2.7, 3.1, and 3.9 ?, respectively, as shown in the inserted table in Fig. 2d. Clues about phase selectivity can be drawn from that lattice and atomic size information. Na and K, which are larger than Li, are relatively close to the anatase (101) lattice unit dimensions but more massive than the rutile (110) lattice gaps. Therefore, Na and K can attack Ti-O?Ti bonds in the anatase phase and break the anatase crystalline into a disordered state. On the other hand, Li atoms can effectively attach to the rutile (110) lattice units, rather than the wider lattice spaces of the anatase (101), and thus successfully reduce only the rutile TiO2phase. In that way, the intrinsic adaptability of Li?EDA to the rutile phase and Na/K?EDA to the anatase phase determine the selectiv?ity of the disordering results.

    故事本來(lái)就是人的一種存在方式,人生無(wú)非是一串串故事的連線。改變單一的敘述方式,筑就高遠(yuǎn)的文化意境,撥動(dòng)微妙的情感心弦,或許,這樣“講故事”才會(huì)由內(nèi)而外煥發(fā)品德的溫暖氣息,使教學(xué)更具有張力與內(nèi)涵。

    Fig. 2 NPT synthesis of BTO and its phase selectivity. a M?EDA electrides reduce pristine TiO2 to BTO under NPT conditions. b Different starting TiO2 phases are selectively reduced/disordered by M?EDA solutions. c Amine solvent investigation to synthesize BTO. Adapted with permission from Ref. [28]. d Proposed mechanism for the BTO phase?selective phenomenon. Adapted with permission from Ref. [28, 29]. e Water contact angle measurements (SEO PHX300) of the original P25 TiO2 and the phase?selectively reduced BTO. f Structure and appearance stability characterization by X?ray powder diffraction (SmartLab JD3643N) and digital photo images

    Furthermore, the M?EDA treatment process is easy to scale up and highly repeatable through the alkali metal stepwise feeding. Using a hydrophilic material is necessary to provide good interfacial contact in many photocatalysis and other real?world applications. As shown in Fig. 2e, a water drop fully spreads on the BTO film, which indicates that BTO is more hydrophilic than pristine P25 TiO2. The excellent hydrophilicity of BTO originates from the enriched surface hydroxyl (OH) groups that appear after the M?EDA reduction. Pristine P25 TiO2has a hydrophobic surface, with a 130° water contact angle, due to the absence of hydro?philic functional groups on its intact TiO2surface. Material stability is another concern for practical applications. BTO has maintained its original disordered/ordered structure and appearance for almost 2.5 years under ambient conditions, as represented in Fig. 2f. Thus, BTO has many advantages, from low?cost production to high potential for many practi?cal applications.

    4 Explored and Potential Applications of BTO

    BTO exhibits strong visible?light (380-740 nm) absorption ability with a narrow optical bandgap (Fig. 1b), efficient photoinduced exciton disassociation with a heterojunction structure [21], and excellent hydrophilicity and stability (Fig. 2e, f). Our group has applied BTO to promote green energy and social sustainability in the field of hydrogenation [21], algae elimination from aquatic ecosystems [31], carbon dioxide (CO2) reduction [28, 32], and visible?light?driven organic synthesis (C-H arylation) [33]. Next, we describe those BTO applications and then propose strategies and directions for further designs and applications of BTO.

    4.1 Explored Photocatalytic Aspects of BTO

    Hydrogen has been deemed a perfect blue energy source that could solve the energy crisis in the twenty?first century. For example, its heating value (141.72 MJ kg?1) is three times higher than gasoline (46.4 MJ kg?1) [34], and it is an extremely abundant material that produces zero pollu?tion and has reproducible capabilities through the water. Solar?driven photohydrogenation has received much atten?tion because of its high sustainability. BTO, as a typical semiconductor material, can be used as a robust hydrogena?tion photocatalyst and has shown a remarkable performance enhancement over P25 and most other reported TiO2mate?rials [21]. The extended light absorption spectrum of BTO covers all solar illumination, which maximizes the quantum efficiency of its photocatalysis process. However, it is not enough to have a favorable light?harvesting ability; a desir?able hydrogenation photocatalyst must also produce effec?tive charge separation through a specific structure designa?tion. As shown in Fig. 3a, BTO retains discrete catalytic redox reaction sites for the reduction of water to hydrogen and methanol sacrificial agent oxidation. The right?side gray Rdis responsible for absorbing enough light irradia?tion and generating the photoinduced electron and holes. Afterward, the adjacent Aoaccepts electrons to trigger water splitting. Compared with the conventional core-shell struc?ture of black TiO2, BTO eliminates the need for electrons to migrate from the core to the interface of the shell and water. Therefore, it greatly reduces the potential for charge recombination. Furthermore, the type II band alignment configuration of BTO assists in exciton dissociation and keeping the effective charges. The open ordered/disordered structure of BTO realized a superior H2production rate of 13.89 mmol h?1g?1with 0.5 wt% Pt and 3.46 mmol h?1g?1without the Pt co?catalyst.

    Algae blooms happen regionally in various brine and river systems, mainly due to water eutrophication induced by human activities, and they damage public health and the social economy [35]. Severe overgrowth of algae can kill aquatic creatures by consuming the limited oxygen dissolved in the water. TiO2, as a typical photocatalyst, can gener?ate reactive oxygen species (ROS), which mainly consist of a hydroxyl radical (·OH) and superoxide anion radicals (·O2?), through photo irradiated hot carriers that attack water molecules. The ROS then remove algae. However, conven?tional TiO2has low efficiency in generating sufficient ROS for algae elimination. Based on our previously obtained photocatalytic hydrogenation experience, we applied BTO to remove Chlamydomonas green algae (Fig. 3b) [31]. We expected that the powerfully wide range of light absorption and effective charge separation properties of BTO would produce an efficient ROS amount. The algae removal test was conducted under both UV and solar light with various types of TiO2. The BTO wiped out all the algae cells within 2-2.5 h, which was the most rapid among the kinds of TiO2tested. Thus, BTO has meaningful roles to play in realizing a sustainable society.

    The photoreduction of CO2into chemical fuels under solar or visible light is supposed to be an excellent way to target both energy and environmental concerns. This so?called artificial photosynthesis strategy has been under study for a while, but desirable conversion selectivity and production yield are still lacking [36]. Moreover, it is quite hard to crack the C = O bonds in the CO2molecule because the dissociation energy demand is high (around 750 kJ mol?1) [37]. The ideal photocatalyst for the CO2reduction reaction (CO2RR) needs a specific configura?tion with an optical band position (especially the CB) that is close to the CO2reduction potential, such as the ? 0.24 VNHEof CO2to CH4or the ? 0.52 VNHEof CO2/CO, and also efficient charge separation with good electron transport. BTO has those structures, so we conducted CO2reduction experiments using BTO(II) under visible light [28] and BTO hybrid materials (BTO(I)/WO3?Ag) under solar light [32]. The BTO(II) reached unprecedented CH4production levels (3.98 μmol g?1h?1), with the highest yield among all the metal (Pt, Ru, W, and Ag)?doped P25 TiO2materials tested. The evident CO2RR ability was conferred by the excellent match between the CB position of BTO(II) (? 0.24 VNHE) and the CO2to CH4potential and the efficient visible?light absorption by the Adwith rapid charge?carrier disassociation (Fig. 3c). Even though BTO(II) offered excellent CO2RR performance, another critical issue for CO2RR, product selectivity, also has to be addressed. Consequently, we designed and constructed BTO(I)/WO3?Ag, a combination material intended to build a particularZ?scheme band structure, as presented in Fig. 3d. The assembledZ?scheme band alignment can maximize the effective potential between a high CB and low VB and then strengthen the catalytic redox power. Notably, the CB position (? 1.55 VNHE) of BTO(I) is close to the CO2to CO potential (Fig. 1b), which contributes to CO production, and higher than the CB of WO3(0.74 VNHE) used to construct theZ?scheme band alignment. In addition, the low difference between the VB of BTO(I) (1.14 VNHE) and the CB of WO3facilitates the flow of excited WO3electrons to BTO(I), thereby reinforcing the number of effective hot electrons. The decorated Ag nano?particles serve as an electron reservoir that can initiate photoelectron production by means of the localized sur?face plasmon resonance effect and further enhance visible?light absorption. When tested, this BTO basedZ?scheme composite produced absolute CO selective?production of 1166.7 μmol g?1h?1at the excellent photocatalytic elec?tron reaction pace of 2333.4 μmol g?1h?1. All in all, BTO showed vigorous CO2RR strength in producing CH4or CO with high output and selectivity, which means it can be an attractive way to tackle global warming and energy deficiency together.

    Fig. 3 Explored photocatalytic applications for BTO. a Unique three?phase?interface BTO(I) robust H2 photogeneration from water. Adapted with permission from Ref. [21]. b Efficient Chlamydomonas green algae disinfection by BTO(I) under solar irradiation. Adapted with permis?sion from Ref. [31]. c Visible?light?driven CO2 reduction (CO2RR) to CH4 by BTO(II). Adapted with permission from Ref. [28]. d BTO(I)/WO3?Ag combination with a Z?scheme band structure for high?selectivity CO2RR to CO. Adapted with permission from Ref. [32]. e BTO(I) photocatalytic activity in C-H arylation organic synthesis. Adapted with permission from Ref. [33]

    Light?driven chemical synthesis is also an essential field that requires promising photocatalysts to boost synthesizing efficiency [38]. C-H arylation for organic synthesis was cho?sen as a typical study case to show the photocatalytic activity of BTO (Fig. 3e) [33]. The phase?mixed BTO absorbs light in the visible range through its Ti3+defect?rich disordered state. It maintains good adsorptivity of an organic reactant and charges separation via its ordered crystalline phase. First, a charge transfer complex (4) formed on the Aosite of BTO(I) from the aryl diazonium compound (2). Then, under visible?light irradiation, photogenerated electrons flowed to the anatase CB due to the type II band alignment and efficiently separated from the holes. An aryl intermedi?ate radical (5) was produced after the single electron transfer process from Aoto (4). As arylation proceeded, after initia?tion by aryl radical (5), the resulting radical (7) intermedi?ate was oxidized by the hot hole carrier from the AoVB and gave the desired product (3) after deprotonation of the product (8). Moreover, BTO offers high reusability through direct filtration, and it maintained consistent yield (63%) performance when five batches were examined under six?fold scaled?up conditions. This application of BTO to pho?tocatalytic chemical synthesis will enrich the role of TiO2in industrial chemical synthesis and contribute to further product cost reductions.

    4.2 Potential Application and Design Commentary of BTO

    Currently, ammonia (NH3) synthesis from nitrogen gas (N2) is an essential approach to supplying nitrogen to plants and humans by industry manufacturing. The Haber-Bosch pro?cess for NH3synthesis (N2+ H2→ NH3), which has been used in industry for more than a century, urgently needs to be replaced due to its high consumption of fossil fuels, which results in enormous greenhouse gas (CO2) emissions and extremely harsh operating conditions (400-500 °C, 100-200 bar with an iron?based catalyst) [39]. Therefore, photocatalysis nitrogen fixation that can use sustainable solar energy and eliminate CO2emissions has attracted growing attention. However, it remains challenging to design an effi?cient photocatalyst to convert N2to NH3under NPT condi?tions with a high production rate and clear mechanism [40]. It has been reported since 1977 that TiO2generated NH3and other gasses under UV irradiation with an N2source, but the process offered minimal yields and low selectiv?ity [41]. After several decades of progress, the yields from TiO2?driven photosynthesis of NH3have been enhanced by hundreds?fold [40]. However, most related studies still apply only UV light because of the narrow light absorption region of conventional TiO2, which hinders the application range and produces low solar coulombic efficiency. As illus?trated in Fig. 4a, by tracking the advanced TiO2photocata?lyst design milestones, it has high credits to investigate the N2fixation to NH3by taking phase?selective disordering and visible?light harvesting advantages of BTO for target?ing maximized NH3production yield and selectively under mild NPT conditions.

    In recent years, volatile organic compounds (VOCs), which vaporize easily at room temperature, have become major hazardous pollutants in the air through speedy indus?trialization and urbanization. Some studies show that indoor atmospheres can have 2-10 times more VOCs than outdoor environments [42]. Therefore, VOCs’ health concerns, such as cancer, headaches, and dizziness, are serious among peo?ple who spend most of their time in buildings or enclosed spaces. Among the various VOCs, toluene, benzene, and aldehydes (formaldehyde and acetaldehyde) are the most common and toxic species [43]. Photodegradation of VOCs is inevitably regarded as the best and most economical choice for dealing with VOCs in the air. The carbon-car?bon bonding and carbonyl groups in VOC molecules are comparatively stable, requiring sufficiently hot carriers from a powerful photocatalyst to be decomposed. BTO is expected to actively cause full VOC degradation into CO2and H2O by effectively generating photoinduced charges and inhibiting exciton recombination under solar and indoor LED lamplight (Fig. 4b). Additionally, the hydroxyl?rich character of the disordered portion of BTO can specifically support the covalent coating and binding process on various substrates and objects (such as air conditioner filters, indoor walls, and subway carriages) and thereby provide versatile application choices.

    Microbial pathogens, which include various bacteria and viruses, are major health concerns to humans world?wide. They occasionally cause serious infectious disease pandemics, such as those caused by the novel corona?virus (COVID?19), severe acute respiratory syndrome coronavirus (SARS), swine influenza virus (H1N1), and Middle?East respiratory syndrome coronavirus (MERS) [16]. For the sake of human health, society needs effec?tive microbial disinfection systems with enough versatility to attack airborne, waterborne, and foodborne pathogenic species. Practically, various microbicidal processes have already been adopted, such as UV disinfection, antibi?otic sterilization, thermal treatments, and nanofiltration. However, the current approaches possess significant limi?tations; for instance, some microbes have already evolved antibiotic or UV resistance [44], and thermal, and filtration operations can cause energy exhaustion and are incompat?ible in many spaces. The microbial pathogens inactivation by TiO2photocatalyst can trace to 1994 after the Sjogren et al. finds the inactivation ability to bacteriophage MS2 on TiO2[45]. Besides, TiO2could be a good option for microorganism disinfection that is low cost, requires mini?mal energy consumption, and is harmless and eco?friendly [46, 47]. In the TiO2photocatalysis microorganism disin?fection process, the ROS generated from photocatalytic processes after light irradiation plays the major roles [16]. To further boost the microbial pathogens inactivation per?formance of TiO2, we need to strengthen the producing amount of ROS species. In the authors’ group previous reports, BTO can generate a higher amount of ROS spe?cies under UV, visible or solar light illumination, which is represented by the higher peak intensity of BTO than pristine TiO2in electron paramagnetic resonance analysis [31, 48]. Therefore, BTO could act as a broad?spectrum antimicrobial agent and outperform pristine TiO2by gen?erating sufficient antibacterial and viricidal ROS at differ?ent band positions, as depicted in Fig. 4c. Harmful bacteria and viruses in living spaces could be effectively deacti?vated under mild conditions by using BTO and solar or visible light.

    Fig. 4 Potential applications and design commentary of BTO. a Photo?driven N2 reduction to NH3 to replace the conventional Haber-Bosch approach. b Photodegradation of volatile organic compounds (VOCs), especially in indoor atmospheres. c Adapting to visible?light?induced microbicidal processes. d Exploring BTO as electrode material in an energy storage system by taking advantage of its electro?conducting Ti3+ species, oxygen vacancy, and stability

    Because TiO2has superior stability, high safety, and good economic value, it has been investigated and considered as an anode or cathode candidate in various ion battery systems, including single?valent alkali?ion batteries (LIBs, SIBs, and KIBs) [49], multivalent magnesium ion batteries (MIBs) [50] and aluminum ion batteries (AIBs) [51]. Also, researchers have noticed that Ti3+self?doped black anatase TiO2has better rate capability than pristine white anatase in LIBs [52], and the associated OV of black TiO2resulted in high?performance magnesium ion (Mg2+) storage [50]. Nevertheless, the synthesis of black TiO2requires a high?temperature reduction process, and their black TiO2prod?ucts remain in a majority crystalline phase and only acquire a small portion Ti3+; even the OV and Ti3+was suggested as main contributions to the advances. Therefore, we pro?pose BTO (including the Adand Rdsynthesized by M?EDA) as an encouraging candidate for battery system electrodes (Fig. 4d). Our M?EDA reduction approach, along with the production of BTO under NPT conditions, can almost completely disorder anatase (Na?EDA) and rutile (Li?EDA) TiO2and deliver sufficient OVs and electro?conducting Ti3+species to enhance energy storage performance.

    5 Prospects and Summary

    The science and technology exploitation has been speeding up in modern society than any other historical era. Based on the invention of BTO, the research progress towards energy and society sustainability can be promoted from diverse aspects. The forthcoming flourishing research suggestions based on the account of BTO achievements are suggested below (Fig. 5).

    1. Design and synthesize a BTO specific morphology and structure in a different dimension (0, 1, 2, 3D). Nano?structured materials are essential for photoelectrochemi?cal devices because of their exposed active surfaces, obviously upgraded kinetics, and versatile adaptations [53]. The potential of BTO could be widely explored by investigating it in 0D (quantum dots), 1D (nanowires, nanotubes, nanoribbons, and nanorods), 2D (nanoplates, nanodisks, and nanosheets), and 3D (nanoflowers, nano?coils, and ordered mesoporous framework) forms.

    Fig. 5 Future research suggestions based on the unique properties of BTO to improve energy and social sustainability

    2. Construct graphene/carbon composites with BTO for use in flexible and wearable energy devices to advance their mechanical and electron flow properties.

    3. Synergize BTO with other typical transition metal dichalcogenides and single or dual metal atoms to further boost its photocatalytic performance in terms of yield, selectivity, and long?term stability.

    4. Couple BTO applications with external fields (elec?tricity, magnetism, plasmonic energy, microwaves, or polarized light). The external fields are expected to influ?ence the photocatalytic process in several ways, such as inducing polarization in reactant molecules (like CO2, N2, and VOCs) to assist in the dissociation of molecules, prompting chiral molecule pure enantiomer synthesis, and altering the hot carrier migration pathways of the photo?catalyst under an electromagnetic wave, so on.

    5. On the frontier of space science, one of the ultimate goals is to build an environment in which humans could live. Space applications of BTO could lead to a bright future for sustainable human civilization. Currently, the International Space Station is equipped with the “Photocatalytic Oxidation Reactor System” (PORS) for VOC removal during the potable water purification step [54]. And the Kennedy Space Center has developed a visible?light?responsive Ag?doped TiO2catalyst PORS in 2016 for better water purification system [55]. BTO, as an advanced photocatalyst, has shown superior pho?tocatalytic activity than most noble metal?doped TiO2and will enable the efficient acquisition of clean?living necessities (food, water, and air) in the Space living area. Furthermore, researchers have found that up to 10 wt% of TiO2exists in the regional area of Moon’s crust, which can further serve to assist the future human exploration of the Moon [56].

    Herein, we have described milestones in TiO2mate?rial design, including the development of BTO. Then, we explained our M?EDA phase?selective disordering mecha?nism and the unique advances offered by BTO in visible?light absorption and exciton disassociation. We continued by discussing applications already achieved and pro?spective advances from those. Last, we proposed several potential new prospects for BTO that target energy and social sustainability. Relying on the structure specialty and superior accomplishments, the unique NPT?synthesized BTO could offer more socially beneficial applications and approach to commercial, robust visible?light?driven ver?satile photocatalyst if its potential is fully explored by the research community.

    AcknowledgementsThis work was supported by the Institute for Basic Science (IBS?R011?D1) and partially supported by the Korea Evaluation Institute of Industrial Technology (20004627) and the INNOPOLIS Foundation (2019?DD?SB?0602).

    Open AccessThis article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons licence, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Com?mons licence, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Com?mons licence and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this licence, visit http://creat iveco mmons.org/licen ses/by/4.0/.

    猜你喜歡
    心弦一串串連線
    快樂(lè)連線
    快樂(lè)連線
    “雞毛蒜皮”也能撩動(dòng)心弦!
    十幾歲(2021年4期)2021-03-31 00:48:58
    快樂(lè)連線
    絲動(dòng)心弦
    一支游子心弦上的小夜曲
    快樂(lè)連線
    心弦上的景致
    腳印一串串等
    午夜福利,免费看| 欧美黑人精品巨大| 午夜日韩欧美国产| 女人爽到高潮嗷嗷叫在线视频| 亚洲欧洲日产国产| 少妇的丰满在线观看| 少妇的丰满在线观看| 亚洲国产av影院在线观看| 国产男女超爽视频在线观看| 他把我摸到了高潮在线观看 | 天天躁狠狠躁夜夜躁狠狠躁| 黑人巨大精品欧美一区二区mp4| 中文字幕av电影在线播放| 亚洲欧洲精品一区二区精品久久久| 日韩有码中文字幕| 美女高潮喷水抽搐中文字幕| 欧美激情久久久久久爽电影 | 母亲3免费完整高清在线观看| 国产高清激情床上av| 国产亚洲av高清不卡| 午夜福利视频精品| 黄色a级毛片大全视频| 久久久久精品国产欧美久久久| 正在播放国产对白刺激| aaaaa片日本免费| 国产国语露脸激情在线看| 日本av免费视频播放| 中文字幕人妻丝袜制服| 亚洲欧美日韩另类电影网站| av电影中文网址| 日日爽夜夜爽网站| 91老司机精品| 18禁美女被吸乳视频| 日韩免费av在线播放| 三上悠亚av全集在线观看| 久久影院123| 国产亚洲精品久久久久5区| 91av网站免费观看| 亚洲精品成人av观看孕妇| 最新美女视频免费是黄的| 亚洲一卡2卡3卡4卡5卡精品中文| 国产午夜精品久久久久久| 久久天堂一区二区三区四区| 国产亚洲精品第一综合不卡| 国产深夜福利视频在线观看| 超碰97精品在线观看| 精品少妇一区二区三区视频日本电影| 欧美精品亚洲一区二区| 一本大道久久a久久精品| 9191精品国产免费久久| 亚洲国产av新网站| 黑丝袜美女国产一区| 日本五十路高清| 在线亚洲精品国产二区图片欧美| 黄网站色视频无遮挡免费观看| 999久久久精品免费观看国产| 另类精品久久| 亚洲国产看品久久| 欧美激情 高清一区二区三区| 一进一出好大好爽视频| 999久久久国产精品视频| 精品国产国语对白av| 黑人欧美特级aaaaaa片| 国产成人av教育| 国产精品 国内视频| 国产免费现黄频在线看| 国产欧美日韩一区二区三| 精品亚洲成国产av| 一区二区三区激情视频| 岛国在线观看网站| 美女福利国产在线| 亚洲欧洲精品一区二区精品久久久| 精品久久久久久电影网| 大陆偷拍与自拍| 亚洲美女黄片视频| 丁香六月天网| 三上悠亚av全集在线观看| 欧美日韩黄片免| 丰满饥渴人妻一区二区三| 侵犯人妻中文字幕一二三四区| 夜夜骑夜夜射夜夜干| 91九色精品人成在线观看| 少妇猛男粗大的猛烈进出视频| 亚洲精品乱久久久久久| 国产精品自产拍在线观看55亚洲 | 成人永久免费在线观看视频 | 欧美黄色片欧美黄色片| 亚洲成人免费av在线播放| 一区二区三区激情视频| 久久婷婷成人综合色麻豆| 中文字幕制服av| 国产无遮挡羞羞视频在线观看| 亚洲专区国产一区二区| 亚洲精品一卡2卡三卡4卡5卡| 欧美国产精品va在线观看不卡| 欧美激情久久久久久爽电影 | 国产成人精品久久二区二区免费| 丝袜美足系列| 亚洲成a人片在线一区二区| 国产精品av久久久久免费| 亚洲伊人色综图| 黑人操中国人逼视频| 黄色片一级片一级黄色片| 精品国产一区二区三区久久久樱花| 国产男靠女视频免费网站| 欧美亚洲日本最大视频资源| 国产亚洲精品一区二区www | 高清av免费在线| 午夜激情久久久久久久| 婷婷丁香在线五月| 精品久久蜜臀av无| bbb黄色大片| e午夜精品久久久久久久| www日本在线高清视频| 天堂8中文在线网| 亚洲欧洲精品一区二区精品久久久| a在线观看视频网站| 欧美日本中文国产一区发布| 成年动漫av网址| 午夜视频精品福利| 日日爽夜夜爽网站| 高清在线国产一区| 国产精品久久电影中文字幕 | 十八禁网站网址无遮挡| 国产淫语在线视频| 啦啦啦免费观看视频1| 亚洲精品在线观看二区| 午夜精品国产一区二区电影| 亚洲欧美精品综合一区二区三区| 九色亚洲精品在线播放| 王馨瑶露胸无遮挡在线观看| 真人做人爱边吃奶动态| 99久久99久久久精品蜜桃| 高清欧美精品videossex| 超碰成人久久| 麻豆成人av在线观看| 黄色a级毛片大全视频| 欧美一级毛片孕妇| 日韩有码中文字幕| 欧美日韩一级在线毛片| 日韩大片免费观看网站| 中文字幕色久视频| 国产欧美日韩综合在线一区二区| 极品教师在线免费播放| 天堂动漫精品| 免费高清在线观看日韩| 亚洲九九香蕉| 1024视频免费在线观看| 99香蕉大伊视频| 亚洲免费av在线视频| 女人精品久久久久毛片| 国产一区二区 视频在线| 国产精品电影一区二区三区 | 99精品久久久久人妻精品| 99久久国产精品久久久| 熟女少妇亚洲综合色aaa.| 黑人欧美特级aaaaaa片| 美女福利国产在线| av一本久久久久| 一区二区av电影网| 久久人妻福利社区极品人妻图片| 欧美黑人精品巨大| 涩涩av久久男人的天堂| 色综合欧美亚洲国产小说| 欧美精品人与动牲交sv欧美| 亚洲视频免费观看视频| 国产亚洲av高清不卡| 国产成人精品久久二区二区免费| 国产精品一区二区在线不卡| 国产成人av激情在线播放| 国产人伦9x9x在线观看| 亚洲中文日韩欧美视频| 我要看黄色一级片免费的| 老司机深夜福利视频在线观看| 欧美日韩精品网址| 悠悠久久av| 国产又爽黄色视频| 欧美在线黄色| 丝瓜视频免费看黄片| 在线观看免费视频日本深夜| 不卡av一区二区三区| 国产在视频线精品| 大片免费播放器 马上看| 国产成人免费无遮挡视频| 人人妻人人添人人爽欧美一区卜| 国产在线精品亚洲第一网站| 久久人人爽av亚洲精品天堂| 一级毛片女人18水好多| 丁香六月欧美| 久久国产亚洲av麻豆专区| 高清欧美精品videossex| 欧美 亚洲 国产 日韩一| 色综合婷婷激情| 久久精品亚洲精品国产色婷小说| 黄色毛片三级朝国网站| 精品少妇内射三级| 丁香六月欧美| 亚洲色图综合在线观看| 国产99久久九九免费精品| 热re99久久国产66热| 色综合婷婷激情| 亚洲精品成人av观看孕妇| 蜜桃国产av成人99| 丝瓜视频免费看黄片| 亚洲国产看品久久| 久久久久精品人妻al黑| 麻豆av在线久日| 免费不卡黄色视频| 国产成人啪精品午夜网站| 激情在线观看视频在线高清 | 欧美乱码精品一区二区三区| 黄色怎么调成土黄色| 亚洲国产欧美日韩在线播放| 中文字幕人妻丝袜一区二区| 大香蕉久久成人网| 在线观看免费高清a一片| www.自偷自拍.com| 99国产综合亚洲精品| 精品久久久久久电影网| 热re99久久国产66热| 国产在线观看jvid| 国产黄色免费在线视频| 午夜免费鲁丝| 乱人伦中国视频| 久久人妻福利社区极品人妻图片| 欧美一级毛片孕妇| 妹子高潮喷水视频| 亚洲av电影在线进入| 18禁裸乳无遮挡动漫免费视频| 免费在线观看视频国产中文字幕亚洲| 天天躁狠狠躁夜夜躁狠狠躁| 天堂中文最新版在线下载| 男人舔女人的私密视频| 久久天堂一区二区三区四区| 最近最新免费中文字幕在线| 亚洲国产av新网站| 久久人人爽av亚洲精品天堂| 亚洲午夜精品一区,二区,三区| 国产一区有黄有色的免费视频| 视频区欧美日本亚洲| 别揉我奶头~嗯~啊~动态视频| 伦理电影免费视频| 亚洲成人免费电影在线观看| 国产精品二区激情视频| 亚洲色图 男人天堂 中文字幕| 夜夜夜夜夜久久久久| av一本久久久久| 国产日韩欧美视频二区| 亚洲国产看品久久| 深夜精品福利| 亚洲av电影在线进入| 纵有疾风起免费观看全集完整版| 亚洲黑人精品在线| 中文字幕人妻熟女乱码| 人人妻人人澡人人看| 午夜激情久久久久久久| 国产一区二区 视频在线| 成人永久免费在线观看视频 | 日韩欧美国产一区二区入口| 精品一区二区三卡| 一二三四社区在线视频社区8| 69av精品久久久久久 | 97人妻天天添夜夜摸| 国产欧美日韩一区二区三区在线| 欧美精品高潮呻吟av久久| 美女高潮喷水抽搐中文字幕| 欧美激情高清一区二区三区| 视频在线观看一区二区三区| 国产成人一区二区三区免费视频网站| 免费久久久久久久精品成人欧美视频| 久久青草综合色| 黄色成人免费大全| 成人国产一区最新在线观看| 人妻 亚洲 视频| 90打野战视频偷拍视频| 一级,二级,三级黄色视频| bbb黄色大片| 国产精品免费大片| 亚洲精品av麻豆狂野| 久久久久网色| 亚洲国产欧美日韩在线播放| 美女午夜性视频免费| 亚洲中文av在线| 亚洲国产欧美一区二区综合| 国产国语露脸激情在线看| svipshipincom国产片| 国产成人免费无遮挡视频| 日韩一区二区三区影片| 免费黄频网站在线观看国产| 99re在线观看精品视频| 国产精品免费一区二区三区在线 | 午夜两性在线视频| 精品亚洲成国产av| 国产欧美日韩一区二区三| 俄罗斯特黄特色一大片| 在线观看免费日韩欧美大片| 亚洲国产av新网站| av一本久久久久| av电影中文网址| 老司机靠b影院| 日韩欧美一区视频在线观看| 免费高清在线观看日韩| 久久精品亚洲av国产电影网| 777米奇影视久久| 久久久久久久久免费视频了| 女性被躁到高潮视频| 极品少妇高潮喷水抽搐| 人妻一区二区av| 国产成人精品无人区| 视频区图区小说| 久久人妻av系列| a级毛片黄视频| 999久久久国产精品视频| 久久久欧美国产精品| 亚洲av电影在线进入| 十八禁人妻一区二区| 首页视频小说图片口味搜索| 丰满少妇做爰视频| 不卡一级毛片| 亚洲精品久久成人aⅴ小说| 极品教师在线免费播放| 欧美人与性动交α欧美精品济南到| 悠悠久久av| av欧美777| 日韩欧美免费精品| 日本wwww免费看| 亚洲欧美日韩高清在线视频 | av有码第一页| 久久精品亚洲av国产电影网| 国产激情久久老熟女| 欧美人与性动交α欧美软件| 成人国产一区最新在线观看| 日本精品一区二区三区蜜桃| 亚洲国产欧美一区二区综合| 亚洲精品乱久久久久久| 夜夜骑夜夜射夜夜干| 91字幕亚洲| 国产欧美日韩精品亚洲av| 欧美在线一区亚洲| 久久精品国产99精品国产亚洲性色 | 中国美女看黄片| 99热网站在线观看| 成人国产av品久久久| 97人妻天天添夜夜摸| 精品亚洲成a人片在线观看| 91精品三级在线观看| 亚洲av国产av综合av卡| 91麻豆av在线| 久久国产亚洲av麻豆专区| 亚洲成人免费电影在线观看| avwww免费| 精品免费久久久久久久清纯 | 18在线观看网站| 高清av免费在线| 日韩中文字幕视频在线看片| 美女国产高潮福利片在线看| 亚洲五月色婷婷综合| 亚洲va日本ⅴa欧美va伊人久久| 精品少妇内射三级| 99国产精品99久久久久| 日日爽夜夜爽网站| 窝窝影院91人妻| 香蕉久久夜色| 欧美 亚洲 国产 日韩一| 日韩免费高清中文字幕av| 久久精品国产综合久久久| 大片免费播放器 马上看| 黄色毛片三级朝国网站| 欧美乱码精品一区二区三区| 久久久国产欧美日韩av| 欧美变态另类bdsm刘玥| 满18在线观看网站| 国产成人欧美在线观看 | 久久久国产成人免费| 最新美女视频免费是黄的| 国产精品1区2区在线观看. | 久久热在线av| 亚洲三区欧美一区| 亚洲成人国产一区在线观看| 天天操日日干夜夜撸| 国产男女内射视频| 国产老妇伦熟女老妇高清| 亚洲美女黄片视频| 精品国产乱码久久久久久男人| 亚洲国产av新网站| 精品少妇内射三级| 日韩制服丝袜自拍偷拍| 亚洲成av片中文字幕在线观看| 国产色视频综合| 最近最新中文字幕大全电影3 | 天天躁狠狠躁夜夜躁狠狠躁| 成在线人永久免费视频| av片东京热男人的天堂| netflix在线观看网站| 99国产极品粉嫩在线观看| 国产三级黄色录像| 视频区图区小说| 男男h啪啪无遮挡| 久久久久久人人人人人| 成年人免费黄色播放视频| 日本撒尿小便嘘嘘汇集6| 中文字幕高清在线视频| 婷婷成人精品国产| 亚洲,欧美精品.| av片东京热男人的天堂| av不卡在线播放| 欧美精品高潮呻吟av久久| 国产av精品麻豆| 菩萨蛮人人尽说江南好唐韦庄| 国产免费视频播放在线视频| 伊人久久大香线蕉亚洲五| 国产精品一区二区在线观看99| 日本一区二区免费在线视频| 成人精品一区二区免费| 久久人人97超碰香蕉20202| 五月开心婷婷网| 久久久精品国产亚洲av高清涩受| 精品高清国产在线一区| 国产深夜福利视频在线观看| 精品国产一区二区三区久久久樱花| 日本撒尿小便嘘嘘汇集6| 国产在视频线精品| 国产在线观看jvid| cao死你这个sao货| 亚洲欧洲精品一区二区精品久久久| 成人特级黄色片久久久久久久 | 欧美老熟妇乱子伦牲交| 中国美女看黄片| 国产麻豆69| av一本久久久久| 精品久久久精品久久久| 国产精品一区二区精品视频观看| 亚洲全国av大片| 日韩欧美一区二区三区在线观看 | 三级毛片av免费| 多毛熟女@视频| 一区二区三区国产精品乱码| 久久精品亚洲熟妇少妇任你| 精品国产亚洲在线| 亚洲欧美色中文字幕在线| 99国产精品免费福利视频| 久久中文字幕人妻熟女| 免费人妻精品一区二区三区视频| 无人区码免费观看不卡 | 亚洲精品一卡2卡三卡4卡5卡| 国产欧美日韩一区二区三区在线| 国产av一区二区精品久久| 亚洲一码二码三码区别大吗| 黄色丝袜av网址大全| 悠悠久久av| 91av网站免费观看| 亚洲欧洲日产国产| 黄色视频在线播放观看不卡| 亚洲成人免费电影在线观看| 国产欧美亚洲国产| 一本—道久久a久久精品蜜桃钙片| 成年版毛片免费区| 成年人免费黄色播放视频| 国产一区二区在线观看av| 免费日韩欧美在线观看| 国产一卡二卡三卡精品| 久9热在线精品视频| 亚洲av成人一区二区三| 精品国产一区二区三区四区第35| 久久精品亚洲av国产电影网| 香蕉久久夜色| 欧美午夜高清在线| 黄色片一级片一级黄色片| 久久久久网色| 国产伦理片在线播放av一区| 女警被强在线播放| 757午夜福利合集在线观看| 一二三四社区在线视频社区8| 夜夜夜夜夜久久久久| 麻豆成人av在线观看| 性高湖久久久久久久久免费观看| 成人三级做爰电影| 美女视频免费永久观看网站| 亚洲精品在线美女| 视频区欧美日本亚洲| 制服人妻中文乱码| 十八禁高潮呻吟视频| 久久天躁狠狠躁夜夜2o2o| 精品少妇内射三级| 国产高清激情床上av| 免费观看a级毛片全部| 久久精品亚洲熟妇少妇任你| 午夜福利,免费看| 免费不卡黄色视频| 日韩中文字幕欧美一区二区| 99国产精品一区二区蜜桃av | 亚洲欧洲精品一区二区精品久久久| 久久久久久久国产电影| 久久免费观看电影| 亚洲午夜理论影院| 欧美老熟妇乱子伦牲交| 性少妇av在线| 麻豆乱淫一区二区| 免费观看人在逋| 黄色a级毛片大全视频| 成年动漫av网址| 99久久精品国产亚洲精品| 一区二区三区激情视频| 少妇裸体淫交视频免费看高清 | 母亲3免费完整高清在线观看| 国产成人免费无遮挡视频| h视频一区二区三区| 精品久久久久久电影网| 亚洲三区欧美一区| 国产成人精品无人区| 国产成人精品久久二区二区免费| 国产伦理片在线播放av一区| 人妻久久中文字幕网| 精品人妻1区二区| 青草久久国产| 99国产精品一区二区三区| 国产精品.久久久| 亚洲精品国产色婷婷电影| 搡老岳熟女国产| 成年人黄色毛片网站| 国产老妇伦熟女老妇高清| 五月开心婷婷网| 中文字幕最新亚洲高清| 丁香欧美五月| 精品国产乱码久久久久久小说| 久久久久久久大尺度免费视频| 男女下面插进去视频免费观看| 国产精品久久久久成人av| 日韩三级视频一区二区三区| 伦理电影免费视频| 欧美在线黄色| 成人国产av品久久久| 国产精品二区激情视频| 日韩中文字幕视频在线看片| 久久久久久久国产电影| 又大又爽又粗| 亚洲va日本ⅴa欧美va伊人久久| 成年人免费黄色播放视频| 伦理电影免费视频| 亚洲精品久久成人aⅴ小说| 国产麻豆69| 丝袜在线中文字幕| 最近最新免费中文字幕在线| 搡老熟女国产l中国老女人| 精品少妇黑人巨大在线播放| 亚洲国产中文字幕在线视频| 丰满饥渴人妻一区二区三| 精品午夜福利视频在线观看一区 | 丰满饥渴人妻一区二区三| 免费观看av网站的网址| 一区二区三区国产精品乱码| 亚洲成人国产一区在线观看| 免费久久久久久久精品成人欧美视频| 欧美av亚洲av综合av国产av| 99香蕉大伊视频| 亚洲熟女毛片儿| 亚洲一区二区三区欧美精品| 1024香蕉在线观看| 香蕉国产在线看| 精品国产亚洲在线| 汤姆久久久久久久影院中文字幕| 变态另类成人亚洲欧美熟女 | 午夜福利视频在线观看免费| 热99re8久久精品国产| 亚洲精品中文字幕在线视频| 高清毛片免费观看视频网站 | 日韩欧美国产一区二区入口| 欧美日韩福利视频一区二区| 超碰97精品在线观看| 免费看十八禁软件| av免费在线观看网站| 国产成人精品无人区| 免费日韩欧美在线观看| 极品教师在线免费播放| 亚洲av成人一区二区三| 久久精品人人爽人人爽视色| 日日摸夜夜添夜夜添小说| 91av网站免费观看| 变态另类成人亚洲欧美熟女 | 国产成人欧美在线观看 | 国产亚洲精品第一综合不卡| 99久久精品国产亚洲精品| 精品人妻1区二区| 性少妇av在线| 十八禁高潮呻吟视频| 性少妇av在线| 国产男靠女视频免费网站| e午夜精品久久久久久久| 丁香六月天网| 亚洲伊人久久精品综合| 99国产极品粉嫩在线观看| 国产精品秋霞免费鲁丝片| 久久精品国产a三级三级三级| 99热国产这里只有精品6| 男人舔女人的私密视频| bbb黄色大片| 久久精品国产a三级三级三级| 日本vs欧美在线观看视频| av线在线观看网站| 三级毛片av免费| 男人舔女人的私密视频| 国产精品秋霞免费鲁丝片| 99久久人妻综合| 亚洲成a人片在线一区二区| 人人妻,人人澡人人爽秒播| 国产一区二区在线观看av| 涩涩av久久男人的天堂| 国产精品亚洲av一区麻豆| 国产在线观看jvid| 午夜激情久久久久久久| 考比视频在线观看| 久久人妻av系列| 一本一本久久a久久精品综合妖精| 人人澡人人妻人| 亚洲熟妇熟女久久|