Constructing a tunable defect structure in TiO<sub>2</sub> for photocatalytic nitrogen fixation

Zhang, Guoqiang; Shan, Chongxin; He, Chuanxin; Zhang, Peixin; Mi, Hongwei

doi:10.1039/c9ta10471b

Cited by 84 publications

(68 citation statements)

References 31 publications

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“…A recent example, Zhang and his coworkers demonstrated that the excess of OVs in TiO 2 increased the adsorption and activation ability of N 2 molecules, but also showed disappointing activity due to the decrease of charge separation efficiency. 74 Excess OVs will become the recombination centers of photocarriers, which will greatly Fig. 7 Schematic illustration of the photocatalytic N 2 fixation model in which water serves as both the solvent and proton source, as well as the reversible creation of light-induced Ovs.…”

Section: Oxygen Vacancymentioning

confidence: 99%

Recent advances in photocatalytic nitrogen fixation: from active sites to ammonia quantification methods

Huang

Gao

et al. 2021

RSC Adv.

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Section: Oxygen Vacancymentioning

confidence: 99%

Recent advances in photocatalytic nitrogen fixation: from active sites to ammonia quantification methods

Huang

Gao

et al. 2021

RSC Adv.

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“…Inspired by this work, Zhang et al have studied the effect of oxygen vacancy concentration on the activity of N 2 fixation by using defect-engineered anatase TiO 2 , which synthesized by a solid phase reduction with NaBH 4 , as a model catalyst. [91] They founded that the sample with optimized oxygen vacancy concentration exhibits a threefold increase in charge separation efficiency and shows enhanced activation ability for N 2 molecules. As a result, a high N 2 photofixation rate of 324.86 µmol g -1 h -1 can be achieved under full spectrum, which is 3.85 times that of pristine anatase TiO 2 .…”

Section: Defect Engineeringmentioning

confidence: 99%

Visible‐Light Responsive TiO₂‐Based Materials for Efficient Solar Energy Utilization

Zhang

et al. 2020

Advanced Energy Materials

150

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currents, geothermal, biomass, and solar, have been developed as alternatives. Among them, solar energy is the most abundant, inexpensive, nonpolluting, and sustainable. [5][6][7][8] Some semiconductors, so called photocatalysts, which possess the capacity to harvest solar energy to drive catalytic reactions for valuable chemical production, have been designed and fabricated to achieve efficient solar energy utilization. [9][10][11][12][13][14][15][16][17][18][19] Typically, TiO 2 is recognized as one of the most promising candidates due to its chemical stability, nontoxicity, and high resistance to photocorrosion. [20][21][22][23][24][25] In general, TiO 2 possesses three major phases, including anatase, rutile and brookite, and many other minor phases, such as monoclinic TiO 2 (B). All of them have wide bandgaps of 3.0-3.2 eV. Hence, TiO 2 can only absorb ultraviolet light (UV), while the visible light accounting for ≈43% of solar energy cannot be utilized. Furthermore, the rapid recombination of photogenerated electrons and holes severely limits its quantum efficiency. Thus, overall photocatalytic activity of TiO 2 is very limited, especially under visiblelight irradiation. [26][27][28] A complete photocatalytic reaction using TiO 2 -based photocatalysts involves three major steps: i) light absorption and The photocatalytic properties of TiO 2 have aroused a broad range of research interest since 1972 due to its abundance, chemical stability, and easily available nature. To increase its overall activity, in the past few decades, much effort has been devoted to the fabrication of advanced TiO 2 -based photocatalysts with visible-light response and these photocatalysts have shown great potential in the field of solar energy utilization. Here, recent progress in the investigation of visible-light responsive TiO 2 -based materials are reviewed. Notably, the fabrication strategies and corresponding chemical/ physical properties of visible-light responsive TiO 2 -based materials are described in detail, with a focus on bandgap engineering and junction engineering from the perspective of light absorption, charge transfer and separation, and surface reactions. Their applications in solar-fuel production, organic synthesis, bacterial disinfection, pollutant degradation and nitrogen fixation are also discussed. Moreover, the new trends and ongoing challenges in this field are proposed and highlighted.

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“…[23] Subsequently, many studies have shown that N 2 chemisorption occurs on OV sites of TiO 2 , which is mainly caused by electron transfer from OVs into the antibonding orbital of N 2 when absorbed on OV sites. [9,12] Due to the high specific surface area and significantly improved charge separation efficiency, its 2D structure has been constructed for efficient photocatalytic N 2 RR. Most importantly, the ultrathin structure of 2D TiO 2 exposes more OVs sites on the edge, which is conducive to the adsorption and activation of N 2 molecules.…”

Section: Tiomentioning

confidence: 99%

Recent Progress in 2D Catalysts for Photocatalytic and Electrocatalytic Artificial Nitrogen Reduction to Ammonia

Zhang

et al. 2021

Advanced Energy Materials

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produce H 2. Therefore, the prospect of NH 3 chemistry is very attractive. However, because nitrogen (N 2) molecules are very stable and difficult to activate, the current NH 3 synthesis process mainly uses the Haber-Bosch reaction which can be realized under high temperature and pressure (300-500 °C, 100-200 atmosphere). [2] This NH 3 synthesis method is energyconsuming and environment-unfriendly, which consumes 3-5% of the global methane and 1-2% of the global energy, and produces 1.6% of the carbon dioxide (CO 2) emissions. [2a] Therefore, developing the green and sustainable NH 3 synthesis approach is very urgent. Catalyst is the key to NH 3 synthesis, and many researchers have been committed to developing catalysts that can operate under normal temperature and pressure. Many plants can convert N 2 in the air into NH 3 fertilizer through nitrogenase, providing nutrients for their own growth. [3] Further study and analysis showed that the nitrogenase mainly contained ferritin and molybdenum-iron protein, which played an important role in the reduction of N 2 molecules. However, due to the slow reaction of nitrogenase in N 2 fixation process, [4] the research is directed to developing other more efficient approaches. For example, photo catalytic and electrocatalytic N 2 reduction reaction (N 2 RR) at room temperature and pressure are more effective methods to convert N 2 into NH 3. [5] Its raw material is H 2 O and N 2 , the overall reaction is 3H 2 O + N 2 → 2NH 3 + 3/2O 2. Only endless solar energy or clean electricity is needed to continuously convert N 2 to NH 3. It is of great significance in energy and environmental protection to convert the clean energy of light and electricity into chemical energy and realize the efficient utilization and transformation of renewable energy. Therefore, it has aroused the widespread interest of scientific researchers. The process of photocatalytic N 2 RR can be divided into two steps. First, photogenerated electrons are excited to the conduction band, leaving photogenerated holes in the valence band. Then some electrons and holes recombine, while the other part migrates to the photocatalysts' surface to participate in the redox process. The H 2 O can be oxidized into O 2 by photogenerated holes, while the N 2 can combine with photogenerated electrons and protons to form NH 3 through a series of reduction steps. The electrocatalytic N 2 RR reactor consists of an electrolytic Photocatalytic and electrocatalytic N 2 reduction reactions (N 2 RR) for NH 3 synthesis from abundant N 2 , H 2 O, solar energy, and renewable electricity is very attractive. 2D catalysts, including photocatalysts (TiO 2 , Bismuthbased materials, layered double hydroxides (LDHs), carbon nitride, Fe@ Graphene, MoS 2 et al.) and electrocatalysts (metal, graphene, carbon, boron nitride (BN), boron carbide (B 4 C), black phosphorus (BP), boron, transitionmetal oxide/sulfide/nitride/phosphide), have emerged as promising candidates for N 2 RR due to their unique physical, chemical and electronic properties. ...

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Constructing a tunable defect structure in TiO₂ for photocatalytic nitrogen fixation

Abstract: This study provides new insights into constructing efficient nitrogen-fixing photocatalysts by optimizing the OV concentration to coordinate the charge separation efficiency and dissociative adsorption capacity of N2.

Cited by 84 publications

References 31 publications

Recent advances in photocatalytic nitrogen fixation: from active sites to ammonia quantification methods

Recent advances in photocatalytic nitrogen fixation: from active sites to ammonia quantification methods

Visible‐Light Responsive TiO₂‐Based Materials for Efficient Solar Energy Utilization

Recent Progress in 2D Catalysts for Photocatalytic and Electrocatalytic Artificial Nitrogen Reduction to Ammonia

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Constructing a tunable defect structure in TiO2 for photocatalytic nitrogen fixation

Abstract: This study provides new insights into constructing efficient nitrogen-fixing photocatalysts by optimizing the OV concentration to coordinate the charge separation efficiency and dissociative adsorption capacity of N2.

Cited by 84 publications

References 31 publications

Recent advances in photocatalytic nitrogen fixation: from active sites to ammonia quantification methods

Recent advances in photocatalytic nitrogen fixation: from active sites to ammonia quantification methods

Visible‐Light Responsive TiO2‐Based Materials for Efficient Solar Energy Utilization

Recent Progress in 2D Catalysts for Photocatalytic and Electrocatalytic Artificial Nitrogen Reduction to Ammonia

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Constructing a tunable defect structure in TiO₂ for photocatalytic nitrogen fixation

Visible‐Light Responsive TiO₂‐Based Materials for Efficient Solar Energy Utilization