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Chinese Journal of Chemistry 2017年第2期35卷 196-202页

作者： Li, Xuedong Zhang, Qinghong Wang, hongzhi Li, Yaogang Donghua Univ Coll Mat Sci & Engn State Key Lab Modificat Chem Fibers & Polymer Mat Shanghai 201620 Peoples R China Donghua Univ Engn Res Ctr Adv Glasses Mfg Technol Shanghai 201620 Peoples R China

Mesoporous （Ga1-xZnx）（N1-xOx） hexagonal nanoplates were prepared by nitridation of layered double hydrox- ides （LDhs） containing Zn2＋ and Ga3＋ ions with different [Zn]/[Ga] ratios. Their specific surface areas ranged from 21.25 to 50.95 m2/g were much higher than those previously reported. The （Ga1-xZnx）（N1-xOx） showed broad visible light absorption and reduced band gaps with increasing Zn content. When [Zn]/[Ga]=2, the （Ga1-xZnx）（N1-xOx） absorbed strongly the light of wavelength less than 525 nm and showed the highest visible light driven 142 production efficiency. After totally repeated runs for 30 h, the h2-production activity of （Ga1-xZnx）（N1-xOx） did not fall off, indicating its good photochemical stability and photocatalytic activity for long time. herein, the results pro- vide new insights into （Ga1-xZnx）（N1-xOx） as high performance photocatalyst and their potential application in visi- ble-light driven water splitting h2 production.

关键词：（Ga1-xZnx）（N1-xOx） photocatalyst visible light h2 production

缺陷工程调控ZnIn_(2)S_(4)纳米片用于增强近红外驱动制氢

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Science China Materials 2024年第6期67卷 1812-1819页

作者：黄元勇杨洪冯硕马畅文曹佩一李菲菲陆欣宇施伟东 College of Environmental and Chemical Engineering Jiangsu University of Science and TechnologyZhenjiang 212003China School of Chemistry and Chemical Engineering Jiangsu UniversityZhenjiang 212013China

近红外(NIR)光驱动水分解产生氢气(h_(2))一直以来都是光催化领域备受关注的问题,但由于其动力学和热力学方面的缺陷,迄今为止仍是一项艰巨的挑战.为了突破这一限制,我们通过简便的水热法设计出了富含硫空位的无贵金属二维(2D)ZnIn_(2)S... 详细信息

近红外(NIR)光驱动水分解产生氢气(h_(2))一直以来都是光催化领域备受关注的问题,但由于其动力学和热力学方面的缺陷,迄今为止仍是一项艰巨的挑战.为了突破这一限制,我们通过简便的水热法设计出了富含硫空位的无贵金属二维(2D)ZnIn_(2)S_(4)-基光催化剂,并首次使用单组分ZnIn_(2)S_(4)-基材料实现了波长大于800 nm的近红外驱动制氢性能.根据价带光谱、紫外-可见-近红外DRS光谱、稳态PL光谱、瞬态光电流响应和EPR表征,我们揭示了存在一个高效的Urbach带尾吸收用于捕获近红外光.硫空位在ZnIn_(2)S_(4)纳米片中的成功构建不仅扩展了光谱吸收范围,而且具有出色的载流子扩散特性和丰富的活性位点.因此,我们的研究结果可能会为未来开发近红外响应的ZnIn_(2)S_(4)-基光催化剂用于实现高效近红外驱动制氢提供一定的指导.

关键词： near-infrared h2 production ZnIn2S4 sulfur va-cancies Urbach tail

Ni2P loading on Cd0.5Zn0.5S solid solution for photocatalytic h2 production and exceptional nitrogen fixation under visible light

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Ni2P loading on Cd0.5Zn0.5S solid solution for photocatalyti...

PtRu nanoparticles supported on noble carbons for ethanol electrooxidation

河南省化学会2016年学术年会

作者： Chunqiu han Zhaoyu Ma Li Jue Liqun Ye haiquan Xie College of Chemistry & Pharmaceutical Engineering Nanyang Normal University

Transition metal phosphide(TMP) was used as cocatalyst to enhance the photocatalytic activity of CdZnS solid solution for photocatalytic h production and nitrogen fixation under visible light irradiation.The NiP/CdZnS photocatalyst was characterized by X-ray diffraction patterns(XRD),transmission electron microscopy(TEM),UV-vis diffuse reflectance spectra(DRS) and X-ray photoelectron spectroscopy(XPS).The photocatalytic data showed that NiP/CdZnS had higher activity than pure CdZnS for photocatalytic h production and photocatalytic dinitrogen(N) fixation in the absence of any scavengers.After 1 h visible light irradiation(λ> 400 nm),the concentration of Nh reached to 101.5 μmol L.And the quantum efficiency at 420 nm monochromatic light reached 4.32%,which much higher than other semiconductors.Time-resolved PL spectra,photocurrent and electrochemical impedance(EIS) spectroscopy revealed that higher photo-induced carrier separation efficiency of NiP/CdZnS.This work introduced CdZnS solid solution photocatalyst to reduce nitrogen,and offered a greenly,economically and efficiently way for nitrogen fixation.

关键词： Cd0.5Zn0.5S solid solution load photocatalytic h2 production nitrogen fixation

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Journal of Energy Chemistry 2022年第3期31卷 168-180,I0006页

作者： Alberto Rodríguez-Gómez Enrico Lepre Luz Sánchez-Silva Nieves López-Salas Ana Raquel de la Osa Faculty of Chemical Sciences and Technologies University of Castilla-La ManchaEnrique Costa Novella Building.Avda.Camilo Jose Cela1213071 Ciudad RealSpain Colloid Chemistry Department Max Planck Institute of Colloids and InterfacesAm Mühlenberg 114476 PotsdamGermany

In this work,three cytosine derived nitrogen doped carbonaceous materials(noble carbons,NCs)with different atomic C/N ratios and porous networks have been synthesized and used as supports for Pt Ru electrocatalysts in the ethanol oxidation reaction(EOR)for clean hydrogen production.Both,the metal phase and the carbon support play critical roles in the electrocatalysts final performance.Lower NPs size distribution was obtained over supports with low atomic C/N ratios(i.e.,4 and 6)and defined porosity(i.e.,1701 m^(2)g^(-1)for Pt Ru/CNZ and 1834 m^(2)g^(-1)for Pt Ru/CLZ,respectively).In contrast,a lower C/N ratio and poor porous network(i.e.,65 m^(2)g^(-1),Pt Ru/CLK)led to the largest particle size and fostered an increase of the alloying degree between Pt and Ru NPs(i.e.,3%for C/N~6 and 28%for C/N~3).Electrochemical active surface area was found to increase with decreasing NPs size and the alloy extent,due to a higher availability of Pt active sites.Accelerated degradation tests showed that Pt Ru/NCs outperform similar to Pt Ru NPs on commercial carbon pointing at the stabilizing effect of NCs.Pt Ru/CNZ exhibited the best electrochemical performance(i.e.,69.1 m A mgPt-1),outperforming Pt Ru/CLZ and Pt Ru/CLK by3-and 9-fold,respectively,due to a suitable compromise between particle sizes,degree of alloy,textural properties and elemental composition.Best anodes were scaled-up to a proton exchange membrane cell and Pt Ru/CNZ was proved to provide the best electrocatalytic activity(262 m A cm^(-2)and low energy requirements),matching the values obtained by the state of the art of EOR electrocatalysts.

关键词： Noble carbon Cytosine h2 production Ethanol electrooxidation PtRu anode PEM cell

Unveiling the role of metallic CoP@Ni_(2)P sea-urchin-like nanojunction as a photothermal cocatalyst for enhancing the h_(2) generation and benzaldehyde formation over CdZnS nanoparticles

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Journal of Materials Science & Technology 2023年第15期146卷 49-60页

作者： Fenghua Wang Jinhe Li Xiaohui Yu hua Tang Jing Xu Lijuan Sun Qinqin Liu School of Materials Science and Engineering Jiangsu UniversityZhenjiang 212013China School of Environmental Science and Engineering Qingdao UniversityQingdao 266071China School of Physics and Electronic Engineering Jiangsu UniversityZhenjiang 212013China

Aiming to develop a photocatalyst that can simultaneously produce valuable chemicals and clean h_(2) fuel for promoting the utilization efficiency of solar energy,herein,a sea-urchin-like CoP@Ni_(2)P binary nanojunction was employed as an efficient photothermal cocatalyst to couple with zero-dimensional CdZnS(CZS)solid solution for achieving superior coordinative redox reaction.The CoP@Ni_(2)P/CZS hybrid displayed a high solar-driven h_(2) generation rate of 40.92 mmol g^(–1) h^(–1) coupling with a benzaldehyde formation rate of 20.33 mmol g^(–1) h^(–1),which was 16.4 and 8.0 times higher than that of bare CZS.Furthermore,the CoP@Ni_(2)P/CZS hybrid also achieved a high photothermal h_(2) production under a broad light range from 420 to 720 nm,and the h_(2) production reached 44.48μmol g^(–1) h^(–1) under the 720 nm light illumination.The enhanced catalytic performance can be ascribed to that the CoP@Ni_(2)P nanojunction with photothermal effect can speed up the separation and transport of carriers,offer more catalytic active sites,and induce an increase in temperature to optimize reaction kinetics.This study may open a facile route to design novel binary metal phosphides with dual functions in photocatalysis for the full exploitation of solar energy.

关键词： h2 production Selective oxidation Photothermal CoP@Ni_(2)P cocatalyst CdZnS solid solution

Improvement strategies for Ni-based alcohol steam reforming catalysts

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Journal of Energy Chemistry 2023年第11期86卷 447-479,I0010页

作者： Alex Desgagnés Ommolbanin Alizadeh Sahraei Maria C.Iliuta UniversitéLaval Département de Génie Chimique1065 Avenue de la MédecineQuébecQC G1V 0A6Canada

Steam reforming(SR)of fossil methane is already a well-known,documented and established expertise in the industrial sector as it accounts for the vast majority of global hydrogen production.From a sustainable development perspective,hydrogen production by SR of biomass-derived feedstock represents a promising alternative that could help to lower the carbon footprint of the traditional process.In this regard,bio-alcohols such as methanol,ethanol or glycerol are among the attractive candidates that could serve as green hydrogen carriers as they decompose at relatively low temperatures in the presence of water compared to methane,allowing for improved h_(2)yields.however,significant challenges remain regarding the activity and stability of nickel-based catalysts,which are most widely used in alcohol SR processes due to their affordability and ability to break C–C,O–h and C–h bonds,yet are prone to rapid deactivation primarily caused by coke deposition and metal particle sintering.In this state-of-the-art review,a portfolio of strategies to improve the performance of Ni-based catalysts used in alcohol SR processes is unfolded with the intent of pinpointing the critical issues in catalyst development.Close examination of the literature reveals that the efforts tackling these recurring issues can be directed at the active metal,either by tuning Ni dispersion and Ni-support interactions or by targeting synergistic effects in bimetallic systems,while others focus on the support,either by modifying acid-base character,oxygen mobility,or by embedding Ni in specific crystallographic structures.This review provides a very useful tool to orient future work in catalyst development.

关键词： h2 production Alcohol steam reforming Ni-based catalysts Catalyst development Sintering Coke formation

highly efficient conversion of surplus electricity to hydrogen energy via polysulfides redox

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The Innovation 2021年第3期2卷 103-108页

作者： Mo Zhang Jing Guan Yunchuan Tu Suheng Wang Dehui Deng State Key Laboratory of Physical Chemistry of Solid Surfaces Collaborative Innovation Center of Chemistry for Energy Materials(iChEM)College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China State Key Laboratory of Catalysis iChEMDalian Institute of Chemical PhysicsChinese Academy of ScienceZhongshan Road 457Dalian 116023China School of Environmental&Municipal Engineering Qingdao University of TechnologyQingdao 266033China

Decoupled electrolysis of water is a promising strategy for peak load regulation of electricity.The key to developing this technology is to construct decoupled devices containing stable redox mediators and corresponding efficient catalysts,which remains a considerable challenge.herein,we designed a high-performance device,using polysulfides as mediators and graphene-encapsulated CoNi as catalysts.It produced h2 with a low potential of 0.82 V at 100 mA/cm^(2),saving 60.2%more energy than direct water electrolysis.The capacity of h2 production reached 2.53105 mAh/cm^(2),which is the highest capacity reported so far.This device exhibited excellent cyclability in 15-day recycle tests,without any decay of performance.The calculation results revealed that the electronic structure of the graphene shell was modulated by the electron transfer from N-dopant and metal core,which significantly facilitated recycle of polysulfides on graphene surfaces.This study provides a promising method for constructing a smart grid by developing efficient decoupled devices.

关键词： peak shaving and valley filling decoupled electrolysis h2 production chainmail catalyst polysulfides redox

Peptide self‐assembly as a strategy for facile immobilization of redox enzymes on carbon electrodes

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Carbon Energy 2023年第11期5卷 15-30页

作者： Itzhak Grinberg Oren Ben‐Zvi Lihi Adler‐Abramovich Iftach Yacoby Department of Oral Biology The Goldschleger School of Dental MedicineFaculty of MedicineTel Aviv UniversityTel AvivIsrael The Center for Nanoscience and Nanotechnology Tel Aviv UniversityTel AvivIsrael The Center for the Physics and Chemistry of Living Systems Tel Aviv UniversityTel AvivIsrael School of Plant Sciences and Food Security The George S.Wise Faculty of Life SciencesTel Aviv UniversityTel AvivIsrael

Redox-enzyme‐mediated electrochemical processes such as hydrogen production,nitrogen fixation,and CO_(2) reduction are at the forefront of the green chemistry revolution.To scale up,the inefficient two‐dimensional(2D)immobilization of redox enzymes on working electrodes must be replaced by an efficient dense 3D system.Fabrication of 3D electrodes was demonstrated by embedding enzymes in polymer matrices.however,several requirements,such as simple immobilization,prolonged stability,and resistance to enzyme leakage,still need to be addressed.The study presented here aims to overcome these gaps by immobilizing enzymes in a supramolecular hydrogel formed by the self‐assembly of the peptide hydrogelator fluorenylmethyloxycarbonyldiphenylalanine.harnessing the self‐assembly process avoids the need for tedious and potentially harmful chemistry,allowing the rapid loading of enzymes on a 3D electrode under mild conditions.Using the[FeFe]hydrogenase enzyme,high enzyme loads,prolonged resistance against electrophoresis,and highly efficient hydrogen production are demonstrated.Further,this enzyme retention is shown to arise from its interaction with the peptide nanofibrils.Finally,this method is successfully used to retain other redox enzymes,paving the way for a variety of enzyme‐mediated electrochemical applications.

关键词： 3D electrode enzymes encapsulation h2 production hydrogenase peptide hydrogel

NiO-CaO materials as promising catalysts for hydrogen production through carbon dioxide capture and subsequent dry methane reforming

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Journal of Energy Chemistry 2017年第5期26卷 942-947页

作者： Alejandra Cruz-hernández J.Arturo Mendoza-Nieto heriberto Pfeiffer Laboratorio de Fisicoquímica y Reactividad de Superficies(LaFReS) Instituto de Investigaciones en MaterialesUniversidad Nacional Autónoma de MéxicoCircuito exterior s/nCiudad UniversitariaDel.CoyoacánCP 04510Ciudad de MéxicoMexico

In this work, CaO-NiO mixed oxide powders were evaluated as consecutive CO;chemisorbents and catalytic materials for hydrogen production thought the Ch;reforming process. Between the NiO impregnated CaO and CaO-NiO mechanical composite, the first one presented better chemical behaviors during the CO;capture and Ch;reforming processes, obtaining syngas（h;+ CO） as final product. Results showed that syngas was produced at two different temperature ranges, between 400 and 600 °C and at T > 800 °C, where the first temperature range corresponds to the Ch;reforming process but the second temperature range was attributed to a different catalytic reaction process: Ch;partial oxidation. These results were confirmed through different isothermal and cyclic experiments as well as by XRD analysis of the final catalytic products, where the nickel reduction was evidenced. Moreover, when a CO-O;flow was used during the carbonation process a triple process was achieved:（i） CO oxidation,（ii） CO;chemisorption and（iii） Ch;reforming. Using this gas flow the hydrogen production was always higher than that obtained with CO;.

关键词： Methane reforming CO2 capture Calcium oxide h2 production NiO supported

Supercritical CO2 produces the visible-light-responsive TiO2/COF heterojunction with enhanced electron-hole separation for highperformance hydrogen evolution

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Nano Research 2020年第4期13卷 983-988页

作者： Lifei Liu Jianling Zhang Xiuniang Tan Bingxing Zhang Jinbiao Shi Xiuyan Cheng Dongxing Tan Buxing han Lirong Zheng Fanyu Zhang Beijing National Laboratory for Molecular Sciences CAS Key Laboratory of ColloidInterface and Chemical ThermodynamicsCASResearch/Education Center for Excellence in Molecular SciencesInstitute of ChemistryChinese Academy of SciencesBeijing 100190China School of Chemical Sciences University of Chinese Academy of SciencesBeijing 100049China Physical Science Laboratory Huairou National Comprehensive Science CenterBeijing 101400China Beijing Synchrotron Radiation Facility(BSRF) Institute of High Energy PhysicsChinese Academy of SciencesBeijing 100049China

To construct the heterojunctions of TiO2 with other compounds is of great importance for overcoming its inherent shortages and improving the visible-light photocatalytic performance.here we propose the construction of TiO2/covalent organic framework(COF)heterojunction with tight connection by a supercritical CO2(SC CO2)method,which helps bridging the transformation paths for photo-induced charge between T i02 and COF.The produced T i02/COF heterojunction performs a h2 evolution of 3,962 nmol·g^-1·h^-1 under visible-light irradiation,which is-25 times higher than that of pure TiO2 and 4.5 folds higher than that of TiO2/COF synthesized by the conventional solvothermal method.This study opens up new possibilities for constructing heterojunctions for solar energy utilization.

关键词： supercritical CO2 covalent organic fram ework(COF) TiO2 h2 production visible light