Abstract:Hydrogen peroxide (H2O2) has received increasing attention because it is not only a mild and environmentally friendly oxidant for organic synthesis and environmental remediation but also a promising new liquid fuel. The production of H2O2 by photocatalysis is a sustainable process, since it uses water and oxygen as the source materials and solar light as the energy. Encouraging processes have been developed in the last decade for the photocatalytic production of H2O2. In this Review we summarize research progr… Show more
“…In addition, the rational fundamental calculations and simulations based on density functional theory (DFT) should be also paid much more attention to, because they cannot only provide a better fundamental understanding of the formation as well photocatalytic mechanism but also guide the design of efficient 2D/2D photocatalysts. Finally, while the researchers explore novel 2D/2D photocatalysts to meet the requirements of highly efficient photocatalytic performance, one should also pay some attention to that there is plenty of space for developing the existing 2D/2D heterostructures for potential photocatalytic applications, e.g., hydrogen peroxide production [240].…”
Two-dimensional/two-dimensional (2D/2D) hybrid nanomaterials have triggered extensive research in the photocatalytic field. The construction of emerging 2D/2D heterostructures can generate many intriguing advantages in exploring high-performance photocatalysts, mainly including preferable dimensionality design allowing large contact interface area, integrated merits of each 2D component and rapid charge separation by the heterojunction effect. Herein, we provide a comprehensive review of the recent progress on the fundamental aspects, general synthesis strategies (in situ growth and ex situ assembly) of 2D/2D heterostructured photocatalysts and highlight their applications in the fields of hydrogen evolution, CO 2 reduction and removal of pollutants. Furthermore, the perspectives on the remaining challenges and future opportunities regarding the development of 2D/2D heterostructure photocatalysts are also presented.
“…In addition, the rational fundamental calculations and simulations based on density functional theory (DFT) should be also paid much more attention to, because they cannot only provide a better fundamental understanding of the formation as well photocatalytic mechanism but also guide the design of efficient 2D/2D photocatalysts. Finally, while the researchers explore novel 2D/2D photocatalysts to meet the requirements of highly efficient photocatalytic performance, one should also pay some attention to that there is plenty of space for developing the existing 2D/2D heterostructures for potential photocatalytic applications, e.g., hydrogen peroxide production [240].…”
Two-dimensional/two-dimensional (2D/2D) hybrid nanomaterials have triggered extensive research in the photocatalytic field. The construction of emerging 2D/2D heterostructures can generate many intriguing advantages in exploring high-performance photocatalysts, mainly including preferable dimensionality design allowing large contact interface area, integrated merits of each 2D component and rapid charge separation by the heterojunction effect. Herein, we provide a comprehensive review of the recent progress on the fundamental aspects, general synthesis strategies (in situ growth and ex situ assembly) of 2D/2D heterostructured photocatalysts and highlight their applications in the fields of hydrogen evolution, CO 2 reduction and removal of pollutants. Furthermore, the perspectives on the remaining challenges and future opportunities regarding the development of 2D/2D heterostructure photocatalysts are also presented.
“…[5,6] In past years the global production of H 2 O 2 exceeded 3million tons for av alue of 4.2 billion US$, and the global demandi sp rojected to rise at ar ate of almost4 -5 %/ year to reach 5.2 milliontons by 2020. [1] The commercially available H 2 O 2 mainly comes from the anthraquinone AO process, which was developedb yR iedl and Pfleiderer at BASF in 1939 and currently accounts for more than 95 %o ft he total H 2 O 2 production.T he AO process em-ploys hydrogen, anthraquinone and air (O 2 )a sr aw materials and Ni or Pd as catalyst, [1,7] and is carried out in organic solvents,w hich makes it inconvenient from the environmental point of view so that other green alternatives are currently under development including photocatalytic [7] and electrocatalytic [8][9][10] H 2 O 2 processes.…”
Carbon materials slightly doped with heteroatoms such as nitrogen (N‐RFC) or sulfur (S‐RFC) are investigated as active catalysts for the electrochemical bielectronic oxygen reduction reaction (ORR) to H2O2. Mesoporous carbons with wide, accessible pores were prepared by pyrolysis of a resorcinol‐formaldehyde resin using a PEO‐b‐PS block copolymer as a sacrificial templating agent and the nitrogen and sulfur doping were accomplished in a second thermal treatment employing 1,10‐phenanthroline and dibenzothiophene as nitrogen and sulfur precursors, respectively. The synthetic strategy allowed to obtain carbon materials with very high surface area and mesopore volume without any further physicochemical post treatment. Voltammetric rotating ring‐disk measurements in combination with potentiostatic and galvanostatic bulk electrolysis measurements in 0.5 m H2SO4 demonstrated a pronounced effect of heteroatom doping and mesopores volume on the catalytic activity and selectivity for H2O2. N‐RFC electrode was employed as electrode material in a 45 h electrolysis showing a constant H2O2 production of 298 mmol g−1 h−1 (millimoles of H2O2 divided by mass of catalyst and electrolysis time), with a faradic efficiency (FE) up to 61 % and without any clear evidence of degradation. The undoped carbon RFC showed a lower production rate (218 mmol g−1 h−1) but a higher FE of 76 %, while the performances drastically dropped when S‐RFC (production rate 11 mmol g−1 h−1 and FE=39 %) was used.
“…3 Substantial efforts have been devoted to the development of effective photocatalysts for the H 2 O 2 generation from water and O 2 . 4 In this photocatalytic process, the sluggish oxidation of water induced by the photogenerated valence holes is a limiting factor for the production of H 2 O 2 . [5][6][7][8][9] Most previous reports focused on improving the half-reaction of O 2 reduction, e. g. by consuming holes with sacri cial agents, such as isopropyl alcohol, benzyl alcohol, and 2-PrOH.…”
Photocatalytic hydrogen peroxide (H2O2) generation represents a promising approach for artificial photosynthesis. However, the sluggish half-reaction of water oxidation significantly limits the efficiency of H2O2 generation. A substitutional reaction of oxidation with accelerated kinetics to produce value-added chemicals holds promise to tackle this challenge. Here, a benzylamine oxidation with more favorable thermodynamics is employed as the half-reaction to couple with H2O2 generation in water by using defective zirconium trisulfide (ZrS3) nanobelts as photocatalyst. The ZrS3 nanobelts with disulfide (S22-) and sulfide anion (S2-) vacancies exhibit an excellent photocatalytic performance for H2O2 generation and simultaneous oxidation of benzylamine to benzonitrile with a high selectivity of > 99%. The S22- vacancies are revealed to facilitate the separation of photogenerated charge carriers. The S2- vacancies can significantly improve the electron conduction, hole extraction, and kinetics of benzylamine oxidation. As a result, the use of defective ZrS3 nanobelts yields a high production rate of 78 and 32 µmol h-1 for H2O2 and benzonitrile, respectively, under a simulated sunlight irradiation.
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