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Journal of Materials Science & Technology 2024年第16期183卷 23-31页

作者： Dehong Yang Yang Li Ruihua Chen Xiangjian Wang Zhi Li Tao Xing Lei Wei Sheng Xu Pengcheng Dai Mingbo Wu College of New Energy State Key Laboratory of Heavy Oil ProcessingChina University of Petroleum(East China)Qingdao 266580China National Engineering Research Center of Coal Gasification and Coal-based Advanced Materials Shandong Energy Group Co.Ltd.Jining 273500China Qinghai Salt Lake Industry Co. Ltd.Haixi Mongolian and Tibetan Autonomous PrefectureQinghai 850099China

The self-assembly of two-dimensional(2D)semiconductor nanosheets into three-dimensional(3D)ordered superstructures represents an ingenious way to avoid aggregation,expose massive available active sites and benefit the mass transfer,which maximizes the advantages of the 2D nanostructures in ***,a flower-like superstructure of ternary semiconducting boron carbon nitride nanosheets(FS-BCNNSs)was synthesized through the morphology-preserved thermal transformation of a flower-like superstructure of boron-containing metal-organic framework nanosheets(FS-MOFNSs).Taking advantage of this functional superstructure,FS-BCNNSs was employed for the pioneering application in the field of photocatalytic hydrogen peroxide(H_(2)O_(2))production and exhibited excellent photocatalytic performance,yielding an impressive rate of 1415.9μmol g^(−1)h^(−1)for the production of H_(2)O_(2).The results of this work offer not just a promising catalyst for photocatalytic H_(2)O_(2)production but also a facile strategy to fabricate unique superstructures constructed from 2D nanosheets for catalysis,energy conversion,and other related fields.

关键词： Photocatalysis Boron carbon nitride Flower-like superstructure Metal-organic framework hydrogen peroxide production

Enhancing photocatalytic hydrogen peroxide production of Tibased metal-organic frameworks:The leading role of facet engineering

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Nano Research 2022年第7期15卷 6045-6053页

作者： Xue-Yang Ji Yao-Yao Wang Yun Li Ke Sun Meng Yu Jun Tao Key Laboratory of Cluster Science of Ministry of Education School of Chemistry and Chemical EngineeringLiangxiang CampusBeijing Institute of TechnologyBeijing 102488China

Rational construction of the facet engineering over metal-organic frameworks is of significant interest for enhancing photocatalytic performance,yet the role of modulator except regulating facet is largely ***,facet engineering of NH_(2)-MIL125(aMIL)was achieved through the facile one-pot method by controlling the concentration of acetic acid *** probable domino effects induced with the detectable modulator were extensively investigated,evidencing the multi-position in one mode contained powder X-Ray diffraction(PXRD),scanning electron microscopy(SEM),X-ray photoelectron spectroscopy(XPS),and X-ray absorption spectroscopy(XAS),***,correlation among the{111}facets engineering,the degree of structural defects,and the performance of photocatalytic hydrogen peroxide(H_(2)O_(2))production was studied in detail,revealing that facet and defect engineering respectively play positive and relatively negative roles in the photocatalytic oxygen reduction reaction(ORR)with a volcano-type ***-3 photocatalyst could deliver H_(2)O_(2) production rate of 925.8μmol·h^(−1)·g^(−1)(2.03-fold of aMIL)under visible-light irradiation and a quantum yield of 1.08%at 420 nm.

关键词： metal-organic frameworks facet engineering defects photocatalyst hydrogen peroxide production

Marrying luminescent metal nanoclusters to C_(3)N_(4) for efficient photocatalytic hydrogen peroxide production

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Materials Reports(Energy) 2024年第2期4卷 83-89页

作者： Zhen Jiang Ziqi Li Qiuxia He Songjie Han Yong Liu Haiguang Zhu Xun Yuan College of Materials Science and Engineering Qingdao University of Science and Technology(QUST)53 Zhengzhou Rd.Shibei DistrictQingdao266042PR China

Photocatalytic oxygen(O_(2))reduction has been considered a promising method for hydrogen peroxide(H_(2)O_(2))***,the poor visible light harvesting and low-efficient separation and generation of charge carriers of conventional photocatalysts strongly limited their photocatalytic H_(2)O_(2) generation ***,we design a highly efficient photocatalyst in this work by marrying luminescent gold-silver nanoclusters(AuAg NCs)to polyethyleneimine(PEI)modified C_(3)N_(4)(C3N4-PEI).The key design in this work is the utilization of highly luminescent AuAg NCs as photosensitizers to promote the generation and separation of charge carriers of C_(3)N_(4)-PEI,thereby ultimately producing abundant e−for O_(2) reduction under visible light illumination(λ≥400 nm).As a result,the as-designed photocatalyst(C3N4-PEI-AuAg NCs)exhibits excellent photocatalytic activity with an H_(2)O_(2) production capability of 82μM in pure water,which is 3.5 times higher than pristine C_(3)N_(4)(23μM).This interesting design provides a paradigm in developing other high-efficient photocatalysts for visible-light-driven H_(2)O_(2) production.

关键词： Visible-light-driven oxygen reduction Metal nanoclusters Graphitic carbon nitride hydrogen peroxide production

Aqueous Synthesis of Covalent Organic Frameworks as Photocatalysts for hydrogen peroxide production

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CCS Chemistry 2022年第12期4卷 3751-3761页

作者： Fanglin Tan Yuanyuan Zheng Zhipeng Zhou Honglei Wang Xin Dong Jing Yang Zhaowei Ou Haoyuan Qi Wei Liu Zhikun Zheng Xudong Chen Key Laboratory for Polymeric Composite and Functional Materials of Ministry of Education School of ChemistryState Key Laboratory of Optoelectronic Materials and TechnologiesSun Yat-sen UniversityGuangzhou 510275 Key Laboratory of Low-Carbon Chemistry&Energy Conservation of Guangdong Province Key Laboratory for Polymeric Composite and Functional Materials of Ministry of EducationSchool of Materials Science and EngineeringSun Yat-sen UniversityGuangzhou 510275 Center for Advancing Electronics Dresden(cfaed)and Faculty of Chemistry and Food Chemistry Technical University of DresdenDresden 01069 Central Facility of Electron Microscopy Electron Microscopy Group of Materials ScienceUniversität UlmUlm 89081 Key Laboratory for Polymeric Composite and Functional Materials of Ministry of Education School of ChemistrySun Yat-sen UniversityGuangzhou 510275

Covalent organic frameworks(COFs)are crystalline porous polymers with designable structures and *** crystallization typically relies on trialand-error experimentation involving harsh conditions,including organic solvents,presenting significant obstacles for rational design and large-scale ***,we present a liquid crystal-directed synthesis methodology and its implementation for up to gram-scale production of highly crystalline COFs in water and *** is compatible with monomers of different structures,shape,size,length of side chains,and electron-donating,electron-accepting,and heterocyclic substitutions near reactive *** types of donor-acceptor two-dimensional COFs including four types of new ones and a three-dimensional COF with a yield of up to 94%were demonstrated,showing great generality of the *** as-synthesized donor-acceptor COFs are organic semiconductors and contain macropores besides intrinsic mesopores which make them attractive *** production of H_(2)O_(2)under visible light in water was studied and the structure-property relationships were *** production rate reached 4347μmol h^(−1)gcat^(−1),which is about 467%better than that of the benchmark photocatalyst g-C_(3)N_(4).This study will inspire the mild synthesis and scale-up of a wide spectrum of COFs and organic semiconductors as efficient catalysts,promote their structure-property investigation,and boost their applications.

关键词： covalent organic frameworks liquid crystal photocatalysis hydrogen peroxide production porous polymer

An efficient strategy for photocatalytic hydrogen peroxide production over oxygen-enriched graphitic carbon nitride with sodium phosphate

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Chinese Journal of Catalysis 2022年第10期43卷 2690-2698页

作者： Yu Zhang Ling Zhang Di Zeng Wenjing Wang Juxue Wang Weimin Wang Wenzhong Wang State Key Laboratory of High Performance Ceramics and Superfine Microstructure Shanghai Institute of CeramicsChinese Academy of SciencesShanghai 200050China Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of SciencesBeijing 100049China School of Chemistry and Materials Science Hangzhou Institute for Advanced StudyUniversity of Chinese Academy of SciencesHangzhou 310024ZhejiangChina

Photocatalytic hydrogen peroxide(H_(2)O_(2))production is a promising strategy to replace the traditional production processes;however,the inefficient H_(2)O_(2) productivity limits its *** this study,oxygen-rich g-C_(3)N_(4) with abundant nitrogen vacancies(OCN)was synthesized for photocatalytic H_(2)O_(2) production.X-ray photoelectron spectroscopy and Fourier-transform infrared spectroscopy indicated that oxygen-containing functional groups(–COOH and C–O–C)were *** paramagnetic resonance confirmed the successful introduction of nitrogen *** exhibited efficient photocatalytic H_(2)O_(2) production performance of 1965μmol L^(−1) h^(−1) in air under visible-light *** high H_(2)O_(2) production was attributed to the enhanced adsorption of oxygen,enlarged specific surface area,and promoted carrier *** increased H_(2)O_(2) production rate(5781μmol L^(−1) h^(−1))was achieved in a Na_(3)PO_(4) *** improved performance was attributed to the changed reactive oxygen ***,the adsorbed PO_(4)^(3−) on the surface of the OCN promoted the transfer of holes to the catalyst surface.•O_(2)−obtained by O_(2) reduction reacted with adjacent holes to generate 1O_(2),which could efficiently generate H_(2)O_(2) with ***,PO_(4)^(3−),as a stabilizer,inhibited the decomposition of H_(2)O_(2).

关键词： Photocatalysis hydrogen peroxide production Graphitic carbon nitride Singlet oxygen Sodium phosphate

Efficient production of hydrogen peroxide in microbial reverse-electrodialysis cells coupled with thermolytic solutions

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Frontiers of Environmental Science & Engineering 2023年第9期17卷 137-146页

作者： Xi Luo Ao Li Xue Xia Peng Liang Xia Huang College of Life and Environmental Sciences Minzu University of ChinaBeijing 100081China State Key Joint Laboratory of Environment Simulation and Pollution Control School of EnvironmentTsinghua UniversityBeijing 100084China Yangtze Ecology and Environment Co. Ltd.Wuhan 430062China

H_(2)O_(2) was produced at an appreciable rate in microbial reverse-electrodialysis cells(MRCs)coupled with thermolytic solutions,which can simultaneously capture waste heat as electrical *** determine the optimal cathode and membrane stack configurations for H_(2)O_(2) production,different catalysts,catalyst loadings and numbers of membrane cell pairs were *** black(CB)outperformed activated carbon(AC)for H_(2)O_(2) production,although AC showed higher catalytic activity for oxygen *** optimum CB loading was 10 mg/cm^(2) in terms of both the H_(2)O_(2) production rate and power *** optimum number of cell pairs was determined to be three based on a tradeoff between H_(2)O_(2) production and capital costs.A H_(2)O_(2) production rate as high as 0.99±0.10 mmol/(L·h)was achieved with 10 mg/cm^(2) CB loading and 3 cell pairs,where the H_(2)O_(2) recovery efficiency was 52±2%and the maximum power density was 780±37 mW/m^(2).Increasing the number of cell pairs to five resulted in an increase in maximum power density(980±21 mW/m^(2))but showed limited effects on H_(2)O_(2) *** results indicated that MRCs can be an efficient method for sustainable H_(2)O_(2) production.

关键词： Microbial reverse-electrodialysis cell hydrogen peroxide production Ammonium bicarbonate Electrolysis cell Optimization

Unveiling the chemistry behind the electrolytic production of hydrogen peroxide by oxygenated carbon

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Journal of Energy Chemistry 2024年第9期96卷 49-58页

作者： Pan Xiang Kunshang Yang Qihao Yang Yang Gao Wenwen Xu Zhiyi Lu Liang Chen Zhiming Wang Ziqi Tian Institute of Fundamental and Frontier Sciences University of Electronic Science and Technology of ChinaChengdu 610054SichuanChina Key Laboratory of Advanced Fuel Cells and Electrolyzers Technology of Zhejiang Province Ningbo Institute of Materials Technology and EngineeringChinese Academy of SciencesNingbo 315201ZhejiangChina Institute for Advanced Study Chengdu UniversityChengdu 610106SichuanChina

Oxygenated carbon materials exhibit outstanding electrocatalytic performance in the production of hydrogen peroxide(H2O2)through a two-electron oxygen reduction *** nature of the active functional group and underlying reaction mechanism,however,remain ***,a comprehensive workflow was established to identify the active sites from the numerous possible *** common hydroxyl group at the notched edge demonstrates a key role in the two-electron *** local chemical environment weakens the binding of OOH intermediate to substrate while enhancing interaction with solution,thereby promoting the H_(2)O_(2)*** increasing pH,the intramolecular hydrogen bond between OOH intermediate and hydroxyl decreases,facilitating OOH ***,the rise in selectivity with increasing potential stems from the suppression of the four-electron *** active site was further validated through *** by theoretical understanding,optimal performance was achieved with high selectivity(>95%)and current density(2.06 mA/cm^(2))in experiment.

关键词： First-principles calculation Oxygen reductionreaction hydrogen peroxide production Fixed-potential method Oxygenated carbon materials

Selective electrochemical production of hydrogen peroxide at zigzag edges of exfoliated molybdenum telluride nanoflakes

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National Science Review 2020年第8期7卷 1360-1366页

作者： Xuan Zhao Yu Wang Yunli Da Xinxia Wang Tingting Wang Mingquan Xu Xiaoyun He Wu Zhou Yafei Li Jonathan N.Coleman Yanguang Li Institute of Functional Nano and Soft Materials (FUNSOM) Jiangsu Key Laboratory for Carbon-Based Functional Materials and Devices Soochow University College of Chemistry and Materials Science Nanjing Normal University College of Material Science and Opto-Electronic Technology University of Chinese Academy of Sciences School of Physical Sciences and CAS Key Laboratory of Vacuum Sciences University of Chinese Academy of Sciences School of Physics CRANN and AMBER Centers Trinity College Dublin

The two-electron reduction of molecular oxygen represents an effective strategy to enable the green, mild and on-demand synthesis of hydrogen peroxide. Its practical viability, however, hinges on the development of advanced electrocatalysts, preferably composed of non-precious elements, to selectively expedite this reaction, particularly in acidic medium. Our study here introduces 2H-MoTe;for the first time as the efficient non-precious-metal-based electrocatalyst for the electrochemical production of hydrogen peroxide in acids. We show that exfoliated 2H-MoTe;nanoflakes have high activity(onset overpotential ～140 mV and large mass activity of 27 A g;at 0.4 V versus reversible hydrogen electrode), great selectivity（H;O;percentage up to 93%） and decent stability in 0.5 M H;SO;. Theoretical simulations evidence that the high activity and selectivity of 2H-MoTe;arise from the proper binding energies of HOO;and O;at its zigzag edges that jointly favor the two-electron reduction instead of the four-electron reduction of molecular oxygen.

关键词： hydrogen peroxide production non-precious-metal-based electrocatalyst molybdenum telluride liquid phase exfoliation zigzag edges

Recent progress in production and usage of hydrogen peroxide

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Chinese Journal of Catalysis 2021年第8期42卷 1241-1252页

作者： Shunichi Fukuzumi Yong-Min Lee Wonwoo Nam Department of Chemistry and Nano Science Ewha Womans UniversitySeoul 03760Korea Graduate School of Science and Engineering Meijo UniversityNagoyaAichi 468-8502Japan Research Institute for Basic Sciences Ewha Womans UniversitySeoul 03760Korea

hydrogen peroxide has attracted increasing interest as an environmentally benign and green oxidant that can also be used as a solar fuel in fuel *** review focuses on recent progress in production of hydrogen peroxide by solar-light-driven oxidation of water by dioxygen and its usage as a green oxidant and *** photocatalytic production of hydrogen peroxide is made possible by combining the e^(-)and 4e-oxidation of water with the e^(-)reduction of dioxygen using solar *** catalytic control of the selectivity of the e^(-)vs.4e-oxidation of water is discussed together with the selectivity of the e^(-)vs.4e-reduction of *** combination of the photocatalytic e^(-)oxidation of water and the e^(-)reduction of dioxygen provides the best efficiency because both processes afford hydrogen *** solar-light-driven hydrogen peroxide production by oxidation of water and by reduction of dioxygen is combined with the catalytic oxidation of substrates with hydrogen peroxides,in which dioxygen is used as the greenest oxidant.

关键词： hydrogen peroxide production Water oxidation Dioxygen reduction Photocatalytic oxygenation Reaction kinetics and mechanism

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High-rate electrochemical H_(2)O_(2) production over multimetallic atom catalysts under acidic–neutral conditions

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Carbon Energy 2024年第1期6卷 44-62页

作者： Yueyu Tong Jiaxin Liu Bing-Jian Su Jenh-Yih Juang Feng Hou Lichang Yin Shi Xue Dou Ji Liang Key Laboratory for Advanced Ceramics and Machining Technology of Ministry of Education School of Materials Science and EngineeringTianjin UniversityTianjinChina Institute for Superconducting and Electronic Materials University of WollongongInnovation CampusNorth WollongongNew South WalesAustralia Department of Electrophysics National Chiao Tung UniversityHsinchuTaiwanChina Shenyang National Laboratory for Materials Science Institute of Metal ResearchChinese Academy of SciencesShenyangLiaoningChina Institute of Energy Materials Science University of Shanghai for Science and TechnologyShanghaiChina

hydrogen peroxide(H_(2)O_(2))production by the electrochemical 2-electron oxygen reduction reaction(2e−ORR)is a promising alternative to the energy-intensive anthraquinone process,and single-atom electrocatalysts show the unique capability of high selectivity toward 2e−ORR against the 4e−*** extremely low surface density of the single-atom sites and the inflexibility in manipulating their geometric/electronic configurations,however,compromise the H_(2)O_(2) yield and impede further performance ***,we construct a family of multiatom catalysts(MACs),on which two or three single atoms are closely coordinated to form high-density active sites that are versatile in their atomic configurations for optimal adsorption of essential*OOH *** them,the Cox–Ni MAC presents excellent electrocatalytic performance for 2e−ORR,in terms of its exceptionally high H_(2)O_(2) yield in acidic electrolytes(28.96 mol L^(−1) gcat.^(−1) h^(−1))and high selectivity under acidic to neutral conditions in a wide potential region(>80%,0–0.7 V).Operando X-ray absorption and density functional theory analyses jointly unveil its unique trimetallic Co2NiN8 configuration,which efficiently induces an appropriate Ni–d orbital filling and modulates the*OOH adsorption,together boosting the electrocatalytic 2e−ORR *** work thus provides a new MAC strategy for tuning the geometric/electronic structure of active sites for 2e−ORR and other potential electrochemical processes.

关键词： hydrogen peroxide production multiatom catalysts operando X-ray adsorption spectrum reaction mechanism tendency structure-property relation