APPLIED CATALYSIS B-ENVIRONMENTAL
·
2021
·
IF 19.503
Yechen Wang,Yaru Wang,Jianjun Zhao,Yiming Xu
Production of H 2 O 2 via semiconductor photocatalysis has received an increasing attention. Herein the effects of cations in perchlorate form and anions in sodium form are examined. Experiment was conducted with Au/WO 3 under visible light in presence of methanol. The production of H 2 O 2 was greatly promoted by A (Ni 2+ , PO 4 3− , CO 3 2− , and F − ), slightly increased by B (SO 4 2− , NO 3 − , Cl − , and ClO 4 − ), greatly inhibited by C (Cu 2+ , and Fe 3+ ), and slightly decreased by Co 2+ . Moreover, the effect of Ni 2+ was weakening by F − , and vice versa. Analysis showed that Ni 2+ was oxidized into Ni 3+ , reactive to methanol, not to water. On Au/WO 3 electrode, anions A inhibited O 2 reduction, and promoted methanol photo-oxidation, while all anions had little influence on the pathway of O 2 reduction. A plausible mechanism is proposed, involving the hole oxidation of anions (not F − ), followed by methanol oxidation. This work highlights the importance of inorganic ions to the selective reduction of O 2 .
研究领域:
光催化
·
环境科学
·
化学
✓ 已验证
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2020
·
IF 16.683
Yechen Wang,Yaru Wang,Jianjun Zhao,Min Chen,Xubo Huang,Yiming Xu
Production of H 2 O 2 via a more economic, green and safe way is challenging. In this work, we report an efficient production of H 2 O 2 from oxygen reduction reaction (ORR) in aqueous solution over a modified WO 3 with Au nanoparticles . Under visible light at wavelengths longer than 420 nm for 5 h, H 2 O 2 measured from WO 3 and Au/WO 3 were 1.07, and 177 μM, respectively. On addition of methanol, H 2 O 2 obtained from WO 3 , Au/WO 3 , and Au/SiO 2 were 8.55, 544, and 0.36 μM, respectively. Photoluminescence and electrochemical measurement revealed that there was an interfacial electron transfer from the excited WO 3 to Au, followed by two-electron reduction of O 2 on Au sites. Under visible light at wavelengths longer than 535 nm, interestingly, H 2 O 2 was also produced from Au/WO 3 (39 μM at 5 h), while the photocurrent of water oxidation on Au/WO 3 was much larger than those on Au/SiO 2 and WO 3 . Clearly, there is also an interfacial electron transfer from the plasmonic Au to WO 3 , followed by ORR to H 2 O 2 , but such a process fails when WO 3 is excited. However, the production of H 2 O 2 on Au/WO 3 was determined by several factors, including Au content, light absorption, and particle size. A maximum H 2 O 2 was observed at an initial pH 3.0 from 0.35 wt% Au/WO 3 , prepared at 400 °C. Moreover, at the same loading on WO 3 , Au was more efficient than Pd, Ag, Pt, Ni, Cu, and Co, while at the same Au loading, WO 3 was more efficient than BiVO 4 and Bi 2 WO 6 . The superior performance of Au/WO 3 is mainly due to its ability to undergo selective ORR to H 2 O 2 , and to release protons into aqueous solution protecting H 2 O 2 from decomposition.
研究领域:
材料科学
·
化学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Yuntao Xu,Yanfei Cao,Li Tan,Qiao Chen,Yuanxing Fang
Photoanodic hydrogen peroxide (H 2 O 2 ) production via water oxidation is limited by low yields and poor selectivity. Herein, four variations of cobalt phosphides, including pristine CoP and Co 2 P crystals, and two mixed-phase cobalt phosphides (CoP/Co 2 P) with different ratios, were applied as co-catalysts on the BiVO 4 (BVO) photoanode to improve H 2 O 2 production. The optimal yield and selectivity were approximately 9.6 µmol‧h −1 ‧cm −2 and 25.2 % at a voltage bias of 1.7 V vs reversible hydrogen electrode (V RHE ) under sunlight illumination, respectively. This performance is approximately 1.8 times that of pristine BVO photoanode. The roles of the Co and P sites were investigated. In particular, the Co site promotes the breaking of one H O bond in water to form OH • radicals, which is the rate-determining step in H 2 O 2 production. The P site plays an important role in the desorption of H 2 O 2 formed from the catalyst, which is responsible for the recovery of fresh catalytic sites. Among the four samples, Co 2 P exhibited the best performance for H 2 O 2 production because it had the highest rate of OH • formation owing to its improved accumulation property. This study offers a rational design strategy for co-catalysts for photoanodic H 2 O 2 production.
研究领域:
材料科学
·
环境科学
·
化学
✓ 已验证
DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Xingyu Zhan,Yunxiong Zeng,Bo Hong,Xinqing Wang,Yingchun Xia
Artificial photosynthesis for H 2 O 2 production through O 2 reduction is a sustainable and cost-effective technology for the scientific and industrial communities. Metal-free polymeric carbon nitride (CN) is a promising visible-light responsive semiconductive material for photocatalytic H 2 O 2 production. However, its inherently disordered and amorphous structure limits its performance improvement due to high photogenerated carrier complexation and sluggish interlayer charge transfer. Here, we report a high-performance S-type heterojunction, composed of CeO 2 coupled with N -vacancy-rich CN (CeO 2 /Nv-CN), that enhances the photocatalysis of H 2 O 2 production under visible light. The prepared CeO 2 /Nv-CN showed an H 2 O 2 generation rate of up to 69.79 mmol·g −1 ·h −1 , 48.80-fold higher than CN and had an apparent quantum yield of 13.8 % at 400 nm. A synergistic effect among CeO 2 , N -vacancies (Nv) and S-type heterojunction is responsible for such an excellent activity, which increased the O 2 and light absorption sites, built rapid charge diffusion channels, and enhanced two-electron O 2 reduction. This work demonstrates the potential of incorporating nanosized CeO 2 with CN to achieve high-performance photocatalytic H 2 O 2 production, opening new avenues for designing highly efficient polymeric composite photocatalysts for energy conservation.
研究领域:
材料科学
·
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED SURFACE SCIENCE
·
2024
·
IF 6.3
Yue An,Yiwei He,Mingtao Li,Wenying Yu,Na Tian,Yihe Zhang,Hongwei Huang
Graphitic phase carbon nitride (g-C 3 N 4 ) is considered one of the most promising catalysts for photocatalytic production of hydrogen peroxide (H 2 O 2 ) due to its green and non-polluting nature and stability. However, the conventional g-C 3 N 4 prepared by direct thermal polymerization has insufficient reaction sites due to its excessive bulk defects derived from incomplete polymerization and low specific surface area, leading to rapid carrier recombination and limited photocatalytic activity. In this work, a series of crystalline g-C 3 N 4 (CN-UxM) with large specific surface areas have been prepared by a molten salt post-treatment strategy with regulating the precursor ratio of urea to melamine . In-situ KPFM, photoelectrochemical experiment and DFT calculation results show that the sample with an optimized urea/melamine ratio of 20 (CN-U20M) has the highest charge separation and transfer efficiency derived from the internal electric field. And its H 2 O 2 production rate under simulated visible light reaches as high as 10.94 mmol∙g −1 ∙h −1 , far exceeding that of most g-C 3 N 4 -based photocatalysts in reported literatures. The present work provides an effective strategy to enhance the photocatalytic activity of g-C 3 N 4 , which is expected to be applied to other organic semiconductor catalytic systems.
研究领域:
材料科学
·
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
ELECTROCHIMICA ACTA
·
2023
·
IF 6.6
Sun Lina,Sun Liping,Huo Lihua,Zhao Hui
The production of hydrogen peroxide (H 2 O 2 ) through electrochemically reducing O 2 in a two-electron pathway is a potential substitute for the traditional process based on anthraquinone. In this paper, F doping is carried out to prepare N and F co-doped porous carbon embedded Co nanoparticles. The electro-catalytic activity for the electrochemical production of H 2 O 2 is systematically investigated. The composite material demonstrates exceptional electro-catalytic selectivity, reaching approximately 92.5%, and shows an ultra-high rate of producing H 2 O 2 in 4021.4 mmol g -1 h -1 at 0.1 V versus RHE in a 0.5 M H 2 SO 4 electrolyte. It is found that the synergetic effect of Co-Nx and F in the composite material result in its exceptional performance. Adding F atom modulates the Zeta potential of the catalyst and alters the electronic configuration around Co-Nx, creating favorable conditions for the uptake of O 2 and consequently forming OOH*. Additionally, the highly electronegative F atom facilitate desorbing OOH* through electrostatic repulsion, preventing any further degradation. In a homemade electrolyzer containing 80 mg L -1 of Rh B, the H 2 O 2 produced in situ in a 0.5 M H 2 SO 4 electrolyte degrades up to 97.76% of Rh B in just 22.5 min, showcasing its potential for practical wastewater treatment applications.
研究领域:
材料科学
·
环境科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Energy Chemistry
·
2025
·
IF 14.9
Xingxing Chen,Yongli Shen,Fan Yang,Shuang Yao,Wen Zhang,Baojuan Xi,Xuguang An,Shenglin Xiong,Jinhua Ye,Changhua An
Solar-driven hydrogen peroxide (H 2 O 2 ) production offers a sustainable and environmentally friendly alternative to the traditional anthraquinone oxidation method. Conjugated polymers (CPs) are emerging as promising photocatalysts for H 2 O 2 production due to their unique electronic, optical properties, and tunable structures. However, the high exciton binding energy of CPs hinders efficient exciton dissociation and charge separation, limiting their photocatalytic performance. In this work, we synthesized scandium (Sc) atoms decorated CPs with enhanced ordered stacking and crystallinity by introducing benzaldehyde as an end-capping reagent. The strong interaction between charged Sc atoms and electrons facilitates exciton dissociation and improves charge transfer capability. Furthermore, the Lewis acidic nature of Sc atoms promotes oxygen adsorption and enhances the stabilization of superoxide anion intermediate ( ∙ O 2 − ). As a result, the as-synthesized photocatalysts exhibit a high H 2 O 2 production rate of 18 μmol h −1 in pure water, which is three times that of pristine CPs. This work provides valuable insights into the design of organic polymer photocatalysts for various photocatalytic reactions.
研究领域:
材料科学
·
环境科学
·
化学
✓ 已验证
产品关联
DOI
高影响因子
Catalysts
·
2022
·Vol. 12
·期 8
·850
·
IF 4.501
Ge Li,Bin Zhou,Ping Wang,Miao He,Zhao Fang,Xilin Yuan,Weiwei Wang,Xiaohua Sun,Zhenxing Li
The two-electron oxygen reduction reaction (2e−ORR) pathway electrochemical synthesis to H2O2has the advantages of low investment and environmental protection and is considered to be a promising green method. Herein, the oxidized Mo2TiC2MXene (O-Mo2TiC2) was successfully synthesized by a facile hydrothermal method as an electrocatalyst in electrocatalytic H2O2production. The O-Mo2TiC2achieved the 90% of H2O2selectivity and 0.72 V vs. RHE of the onset potential. Moreover, O-Mo2TiC2showed high charge transfer ability and long-term stable working ability of 40 h. This significantly enhanced electrocatalytic H2O2production capacity is assigned the oxidation treatment of Mo2TiC2MXene to generate more oxygen-containing groups in O-Mo2TiC2. This work provides a promising catalyst candidate for the electrochemical synthesis of H2O2.Keywords:two-electron oxygen reduction reaction;electrochemical H2O2production;Mo2TiC2MXene;oxidation treatment
研究领域:
电化学
·
材料科学
·
催化
✓ 已验证
产品关联
DOI
高影响因子
Nature Communications
·
2023
·Vol. 14
·期 1
·1-10
·
IF 16.6
Du Jiannan,Han Guokang,Zhang Wei,Li Lingfeng,Yan Yuqi,Shi Yaoxuan,Zhang Xue,Geng Lin,Wang Zhijiang,Xiong Yueping,Yin Geping,Du Chunyu
The two-electron oxygen reduction reaction in acid is highly attractive to produce H 2 O 2 , a commodity chemical vital in various industry and household scenarios, which is still hindered by the sluggish reaction kinetics. Herein, both density function theory calculation and in-situ characterization demonstrate that in dual-atom CoIn catalyst, O-affinitive In atom triggers the favorable and stable adsorption of hydroxyl, which effectively optimizes the adsorption of OOH on neighboring Co. As a result, the oxygen reduction on Co atoms shifts to two-electron pathway for efficient H 2 O 2 production in acid. The H 2 O 2 partial current density reaches 1.92 mA cm −2 at 0.65 V in the rotating ring-disk electrode test, while the H 2 O 2 production rate is as high as 9.68 mol g −1 h −1 in the three-phase flow cell. Additionally, the CoIn-N-C presents excellent stability during the long-term operation, verifying the practicability of the CoIn-N-C catalyst. This work provides inspiring insights into the rational design of active catalysts for H 2 O 2 production and other catalytic systems.
研究领域:
化学催化
·
材料科学
·
能源化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ENVIRONMENTAL RESEARCH
·
2025
·
IF 7.7
Fanbin Zhang,Xia Qin,Cuicui Xu,Xiyang Li,Hongyun Ren,Xingwei Tao,Xujie Lan
A novel self-breathing gas diffusion electrode was developed by loading carbon nanotubes (CNTs) and carbon black (CB) onto the surface of graphite felt through vacuum filtration. This electrode features a well-structured mesoporous network and a stable three-phase interface, which enable efficient oxygen mass transfer and enhance the self-breathing capability. The incorporation of carbon nanotubes and carbon black significantly boosts the electrode's catalytic performance. In a dual-chamber reactor operating at a current density of 12 mA/cm 2 and an initial pH of 3, the system achieved an H 2 O 2 concentration of 4,691 mg/L within 1 hour, with an energy consumption of 6.58 kWh/kg H 2 O 2 substantially outperforming conventional gas diffusion electrodes. The dynamic pH regulation in the dual-chamber system optimizes the 2e - ORR pathway, leading to corresponding changes in proton transfer pathways and adsorbed species within the Helmholtz plane. Additionally, the presence of reactive hydrogen (H*) enhances the chemisorption of O 2 and facilitates its hydrogenation to form the *OOH intermediate. The electrode exhibited excellent stability, maintaining H 2 O 2 yields above 4000 mg/L over 5 cycles and nearly complete degradation of the simulated contaminants within 30 min in an electro-Fenton system application. These results highlight the electrode's potential for efficient H 2 O 2 synthesis and environmental remediation.
研究领域:
环境科学
·
材料科学
·
电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Xinping Hou,Kai Wang,Jun Wang,Jianhua Yang,Guixin Dong,Shaomin Liu
Piezocatalysis has emerged as a sustainable alternative for hydrogen peroxide production. However, the current development of efficient piezocatalysts is predominantly focusing on those conventional piezoelectric ceramic oxides with high permittivity and limited catalytic activities. Therefore, innovative approaches to develop novel piezocatalysts in particular from these outstanding paraelectric semiconductors are highly required. In this work, by employing a feasible doping strategy, robust piezoelectric property is created on the Ba 2 Nb 2-x Fe x O 6-δ double perovskite oxides, typically characterized by a stable paraelectric cubic structure. Optimum Fe doping not only intensifies the double perovskite phase but also inspires a phase transition from a centrosymmetric cubic to a piezoelectric tetragonal phase, thereby achieving desirable piezoelectricity and enabling a series of favorable physical properties including redox activity, active sites of anion defects, reduced bandgap, and increased free charge density. All these are important factors to enhance piezocatalytic activity. As a result, Ba 2 NbFeO 6-δ achieved by the optimum Fe doping demonstrated exceptional piezocatalytic H 2 O 2 yield of 512 and 690 µmol g -1 h −1 under atmosphere and oxygen-purging conditions, respectively, without the presence of any sacrificial agents. Mechanistic investigations reveal that both water oxidation and oxygen reduction involve in the H 2 O 2 production, wherein piezopotential plays a critical role not only in facilitating the charge carrier separation and transportation but also in modulating the band structure to enhance the catalyst redox capacity. This study offers a feasible and universal strategy for the design of novel piezocatalysts, expanding the windows for catalyst selection for piezocatalysis.
研究领域:
材料科学
·
环境科学
·
化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Binrong Li,Na Li,Zhiwei Guo,Chen Wang,Xuedong Wang,Zhi Zhu,Xu Tang,Pengwei Huo
Polymeric carbon nitride (PCN) is an environmentally friendly photocatalyst for solar-driven H 2 O 2 production, but the activity of original PCN is still not satisfactory. The main limitation is the sluggish exciton dissociation leading to slow generation and conversion of superoxide radical (•O 2 − ) intermediate. Herein, the PCN with dual defect sites and compact interlayer is rationally designed for H 2 O 2 photosynthesis with an ultrahigh rate of 3930.9 μmol g −1 h −1 and rapid •O 2 − yield rate of 1.92 min −1 . The enhanced activity is attributed to effective exciton dissociation during interlayer and intralayer process. Moreover, nitrogen vacancies change the oxygen adsorption configuration (formation of C − O − O − C bridge mode), thus promoting O 2 adsorption and activation. A well-matched linear relationship was established between the concentration of nitrogen vacancies and •O 2 − /H 2 O 2 production. This work not only provides in-depth insights for the photocatalytic H 2 O 2 generation mechanism, but also offers a new paradigm for designing efficient PCN-based photocatalysts for energy conversion.
研究领域:
材料科学
·
光催化
·
能源转换
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）