Trace water triggers high-efficiency photocatalytic hydrogen peroxide production

Xu, Zaixiang; Li, Yang; Cao, Yongyong; Du, Renfeng; Bao, Zhikang; Zhang, Shijie; Shao, Fangjun; Ji, Wenkai; Yang, Jing; Zhuang, Guilin; Deng, Shengwei; Yao, Zihao; Zhong, Xing; Wang, Jianguo

doi:10.1016/j.jechem.2021.03.055

Cited by 38 publications

(32 citation statements)

References 60 publications

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“…To address these bottlenecks, various materials as favorable photoanode, such as TiO 2 , BiVO 4 , WO 3 , Fe 2 O 3 , TaON, Ta 3 N 5 , GaP, etc., have attracted more attention for PEC water splitting. Among different photoanodes, BiVO 4 has been shown to be one of the most promising candidates due to its suitable bandgap and low cost. , However, the PEC performance is restrained by the poor charge transport and serious photocorrosion of BiVO 4 photoanode. , Consequently, extensive efforts have been devoted to addressing the limitations by morphology engineering, heterojunction construction, and surface modification. − Thus, it is inevitable to rationally design excellent and stable BiVO 4 photoanode by effective approach.…”

Section: Introductionmentioning

confidence: 99%

Engineering Single-Atomic Ni-N₄-O Sites on Semiconductor Photoanodes for High-Performance Photoelectrochemical Water Splitting

et al. 2021

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Direct photoelectrochemical (PEC) water splitting is a promising solution for solar energy conversion; however, there is a pressing bottleneck to address the intrinsic charge transport for the enhancement of PEC performance. Herein, a versatile coupling strategy was developed to engineer atomically dispersed Ni-N 4 sites coordinated with an axial direction oxygen atom (Ni-N 4 -O) incorporated between oxygen evolution cocatalyst (OEC) and semiconductor photoanode, boosting the photogenerated electron−hole separation and thus improving PEC activity. This state-ofthe-art OEC/Ni-N 4 -O/BiVO 4 photoanode exhibits a record high photocurrent density of 6.0 mA cm −2 at 1.23 V versus reversible hydrogen electrode (vs RHE), over approximately 3.97 times larger than that of BiVO 4 , achieving outstanding long-term photostability. From X-ray absorption fine structure analysis and density functional theory calculations, the enhanced PEC performance is attributed to the construction of single-atomic Ni-N 4 -O moiety in OEC/BiVO 4 , facilitating the holes transfer, decreasing the free energy barriers, and accelerating the reaction kinetics. This work enables us to develop an effective pathway to design and fabricate efficient and stable photoanodes for feasible PEC water splitting application.

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Section: Introductionmentioning

confidence: 99%

Engineering Single-Atomic Ni-N₄-O Sites on Semiconductor Photoanodes for High-Performance Photoelectrochemical Water Splitting

et al. 2021

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“…Moreover, the H2O2 concentration in the separated aqueous phase achieved during photocatalysis with KPHI-HMDS after 72 h irradiation is ~0.12 M. To the best of our knowledge, such a high value has never been reported for any other light-driven H2O2 production systems in which the obtained H2O2 would be already separated from electron donor as well as from the photocatalyst. 14,64 This impressively demonstrates the advantage of performing the conversion using a hydrophobized photocatalyst in a biphasic system.…”

Section: Photocatalytic H2o2 Production By Hydrophilic and Hydrophobi...mentioning

confidence: 82%

Hydrophobized Poly(Heptazine Imide) for Highly Effective Photocatalytic Hydrogen Peroxide Production in a Biphasic Fatty Alcohol-Water System

Krivtsov

Vazirani²,

Mitoraj³

et al. 2022

Preprint

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Light-driven production of hydrogen peroxide via selective dioxygen reduction is an attractive “green” alternative to the conventionally used anthraquinone process. One of the most promising classes of photocatalytic materials for this conversion that excels by high selectivity, chemical stability and low cost is represented by polymeric carbon nitrides, and particularly by various types of poly(heptazine imide) (PHI), i.e., ionic variants of carbon nitride. A crucial challenge highlighted by recent studies is the problem of separation of formed H2O2 from the reaction medium and especially from the suspended photocatalyst particles since photocatalytically generated H2O2 can undergo light-driven decomposition, as well as disproportionation on the surface of the photocatalyst in the dark. Herein, we report an elegant solution to this problem by implementing a biphasic reaction system in which the hydrophobic photocatalyst oxidizes a lipophilic electron donor in the organic phase, while the produced H2O2 is instantaneously extracted into the aqueous layer. To this end, we have achieved an effective hydrophobization of ionic carbon nitride (PHI) nanoparticles in the form of a composite with alkylated silica. The hydrophobized composite effectively photocatalyzes the reduction of dioxygen to H2O2 with concurrent oxidation of a model fatty alcohol (1-octanol) in the organic phase under visible light irradiation (406 nm LED), and enables, at the same time, facile separation of the high-value H2O2/water mixture from the reaction medium at H2O2 concentrations (~0.12 M) that are unprecedentedly high for light-driven systems reported in the literature. Notably, fatty alcohols are readily available from vegetable waxes and as pulping sub-products, and the products of their partial oxidation represent a valuable feedstock for the synthesis of pharmaceuticals and cosmetic products. This work thus showcases a rational design of a high-performance photocatalytic system for H2O2 production that enables easy separation of the product from electron donors and its recovery at high concentrations, and paves the way for sustainable and economically viable light-driven H2O2 production from easily available feedstock.

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“…Photocatalysis, converting inexhaustible solar energy resources into valuable chemicals, is a promising route for the generation of H 2 O 2 . 2 In the past few years, great efforts have been made to achieve photocatalytic production of H 2 O 2 based on various photocatalysts, such as titanium dioxide (TiO 2 ), [7][8][9] carbon nitride (C 3 N 4 ), [10][11][12][13][14] bismuth vanadate (BiVO 4 ), 15 and metal-organic frameworks (MOFs). 16,17 However, the wide band gap of the above photocatalysts greatly limits their light absorption in a narrow region of the solar spectrum, missing most parts of the visible-light.…”

Section: Introductionmentioning

confidence: 99%

High-efficiency visible-light photocatalytic H₂O₂ production using CdSe-based core/shell quantum dots

Zhang

et al. 2022

Catal. Sci. Technol.

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Trace water triggers high-efficiency photocatalytic hydrogen peroxide production

Cited by 38 publications

References 60 publications

Engineering Single-Atomic Ni-N₄-O Sites on Semiconductor Photoanodes for High-Performance Photoelectrochemical Water Splitting

Engineering Single-Atomic Ni-N₄-O Sites on Semiconductor Photoanodes for High-Performance Photoelectrochemical Water Splitting

Hydrophobized Poly(Heptazine Imide) for Highly Effective Photocatalytic Hydrogen Peroxide Production in a Biphasic Fatty Alcohol-Water System

High-efficiency visible-light photocatalytic H₂O₂ production using CdSe-based core/shell quantum dots

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Trace water triggers high-efficiency photocatalytic hydrogen peroxide production

Cited by 38 publications

References 60 publications

Engineering Single-Atomic Ni-N4-O Sites on Semiconductor Photoanodes for High-Performance Photoelectrochemical Water Splitting

Engineering Single-Atomic Ni-N4-O Sites on Semiconductor Photoanodes for High-Performance Photoelectrochemical Water Splitting

Hydrophobized Poly(Heptazine Imide) for Highly Effective Photocatalytic Hydrogen Peroxide Production in a Biphasic Fatty Alcohol-Water System

High-efficiency visible-light photocatalytic H2O2 production using CdSe-based core/shell quantum dots

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Engineering Single-Atomic Ni-N₄-O Sites on Semiconductor Photoanodes for High-Performance Photoelectrochemical Water Splitting

Engineering Single-Atomic Ni-N₄-O Sites on Semiconductor Photoanodes for High-Performance Photoelectrochemical Water Splitting

High-efficiency visible-light photocatalytic H₂O₂ production using CdSe-based core/shell quantum dots