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Amorphous hybrid tungsten oxide–nickel hydroxide nanosheets used as a highly efficient electrocatalyst for hydrogen evolution reaction

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Nano Research 2024年第4期17卷 2499-2508页

作者： Chao Lyu Chenghai Dai Yiwei Tan State Key Laboratory of Materials-Oriented chemical engineering School of Chemistry and Chemical EngineeringNanjing Tech UniversityNanjing 211816China

There are more challenges for alkaline hydrogen evolution reaction(HER)via simultaneously expediting the electron-coupled water dissociation process(Volmer step)and the following electrochemical H_(2. desorption(Heyrovsky step).Hybrid amorphous electrocatalysts are highly desirable for efficient hydrogen evolution from water-alkali electrolyzers due to the bifunctionality for the different elementary steps of HER and optimal interactions with water molecules and the reactive hydrogen intermediates(Had).Herein,the synthesis of amorphous hybrid ultrathin(tungsten oxide/nickel hydroxide)hydrate(a-[WO_(3)/Ni(OH)_(2.]·0.2._(2.O)nanosheets on nickel foam(NF)for efficient alkaline HER is *** structural and composition features of a-[WO_(3)/Ni(OH)_(2.]·0.2._(2.O are characterized in *** resulting a-[WO_(3)/Ni(OH)_(2.]·0.2._(2.O/NF electrocatalyst with the synergistic effect of both hybrid components for the HER elementary steps shows greatly improved the activity and durability for the HER with a low overpotential of-41 and-163 mV at-10 and-500 mA·cm^(-2.,respectively,a Tafel slope as low as-72.9 mV·dec^(-1),and long-term stability of continuous electrolysis for at least 150 h accompanying by inappreciable overpotential change in 1 M *** the hybrid a-[WO_(3)/Ni(OH)_(2.]·0.2._(2.O,Ni(OH)_(2. and WO_(3) moieties are separately responsible for accelerating dissociative adsorption of water and weakening Had adsorption strength,which is beneficial to the improvement of the alkaline HER activity.

关键词： amorphous nanomaterial bimetallic electrocatalyst tungsten oxide ultrathin nanosheet hydrogen evolution reaction

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Two-dimensional C_(2.N-based single-atom catalyst with complex microenvironment for enhanced electrochemical nitrogen reduction:A descriptor-based design

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Journal of Energy chemistry 2024年第10期97卷 110-119,I0003页

作者： Enduo Dai Wei An Ruixian Guo Xugen Shi Yunyi Li Yibo Wang Mingming Liu College of chemistry and chemical {2..Shanghai University of {2. Science Shanghai 201620China

The catalytic descriptor with operational feasibility is highly desired towards rational design of high-performance catalyst especially the electrode/electrolyte solution interface working under mild ***,we demonstrate that the descriptorΩparameterized by readily accessible intrinsic properties of metal center and coordination is highly operational and efficient in rational design of single-atom catalyst(SAC)for driving electrochemical nitrogen reduction(NRR).Using twodimensional metal(M)-B_(x)P_(y)S_(z)N_m@C_(2.N as prototype SAC models,we reveal that^(*)N_(2.+(H~++e~-)→^(*)N_(2.H acts predominantly as the potential-limiting step(PLS)of NRR on M-B_(2.P_(2.S_(2.@C_(2.N and M-B_(1)P_(1)S_(1)N_(3)@C_(2.N regardless of the distinction in coordination *** the 2. screened M active sites,withΩvalues close to the optimal 4,M-B_(2.P_(2.S_(2.@C_(2.N(M=V(Ω=3.53),Mo(Ω=5.12.,and W(Ω=3.92.)and M-B_(1)P_(1)S_(1)N_(3)@C_(2.N(M=V(Ω=3.00),Mo(Ω=4.34),and W(Ω=3.32.)yield the lowered limiting potential(U_(L))as-0.45,-0.54.-0.36,-0.58,-0.2.,and-0.2. V,respectively,thus making them the promising NRR *** importantly,these SACs are located around the top of volcano-shape plot of U_(L) versusΩ,re-validatingΩas an effective descriptor for accurately predicting the high-activity NRR SACs even with complex *** study unravels the relationship between active-site structure and NRR performance via the descriptorΩ,which can be applied to other important sustainable electrocatalytic reactions involving activation of small molecules viaσ-donation andπ^(*)-backdonation mechanism.

关键词： Electrocatalysis N_(2. reduction Single-atom catalyst Descriptor DFT

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An aqueous rechargeable Fe//LiMn_(2.O_()hybrid battery with superior electrochemical performance beyond mainstream Fe-based batteries

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Nano Research 2024年第6期17卷 5168-5178页

作者： Yu Liu Dehui Xie Yuxin Shi Rongguan Lv Yingna Chang Yuzhen Sun Zhiyuan Zhao Jindi Wang Kefan Song Huayu Wu Tuan K.A.Hoang Rong Xing Huan Pang Institute of New Energy on chemical Storage and Power Sources School of Chemical and Environmental EngineeringYancheng Teachers UniversityYancheng 224000China School of chemistry and chemical {2. Yangzhou UniversityYangzhou 225009China department of chemical {2. University of Waterloo200 University Avenue WestWaterlooOntario N2L 3G1Canada

Aqueous rechargeable batteries(ARBs)are generally safer than non-aqueous analogues,they are also less-expensive,and more friendly to the ***,the inherent disadvantage of the narrow electrochemical window of H2. seriously restricts the energy density and output voltage of ARBs,especially aqueous rechargeable Fe-based ***,we introduce a new battery system:the anode contains C@Fe/Fe_(2.O_(3)composite,which is interfaced with an alkaline electrolyte;the cathode contains LiMn_(2.O_()in contact with a neutral electrolyte.A Li^(+)-conducting membrane is carefully selected to decouple the electrode-electrolyte,which effectively widens the electrochemical window to above 2.65 V,thereby enables an aqueous rechargeable iron *** average output voltage is 1.83 V and its energy density is 2.5.3 Wh/kg at 549 W/*** this work,we propose the energy storage mechanism with the aid of density functional theory(DFT).The calculated reduction potential of the anode agrees with the experimental ***,this battery system demonstrates long cycle lifespan of approximately 2.00 cycles at 2.A/g,corresponding to a capacity retention of 82.1%.These results are very far superior than those of mainstream aqueous rechargeable Fe-based batteries,which guarantee future investigation for storing electricity energy.

关键词： aqueous battery high voltage high energy iron oxide theoretical calculation

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Monomeric and self-assembled crystal phases of TNBT

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Rare Metals 2024年第10期43卷 5442-5448页

作者： Yun-Hui Wu Hua-Bei You Wei-Kai Cui Zhi-Qian Cao Xiao Dong Zi-Hui Meng Ming Huang School of chemistry and chemical {2. Beijing Institute of Technology Institute of chemical Materials China Academy of Engineering Physics

（3,3′,5,5′-Tetranitro-4,4′-bi-1,2.4-Triazole） TNBT was designed and predicted more than three decades ago as a high energy *** with many other designed molecules,TNBT has not been successfully synthesized and has not been computationally studied in *** this work,theoretical calculations at density functional theory （DFT）level of theory were carried out for both the gas phase molecule and its possible bulk crystal *** （DFT） computations show that TNBT is comparable to CL-2. with high bulk density,

关键词： Density functional theory

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Supramolecular Macrocycle Regulated Single-Atom MoS2.Co Catalysts for Enhanced Oxygen Evolution Reaction

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Energy & Environmental Materials 2024年第5期7卷 287-295页

作者： Shuai Cao Wenzhuo Wu Chaozhong Liu Leqian Song Qun Xu Huacheng Zhang Yanli Zhao School of chemical engineering and Technology Xi’an Jiaotong University Henan Institute of Advanced Technology Zhengzhou University department of Materials Science and engineering Zhengzhou University School of chemistry Chemical Engineering and Biotechnology Nanyang Technological University

The development of active water oxidation catalysts for water splitting has stimulated considerable interest. Herein, the design and building of single atom Co sites using a supramolecular tailoring strategy are reported, that is,the introduction of pillar[4]arene[1]quinone （P4A1Q） permits mononuclear Co species stereoelectronically assembled on MoS2.atrix to construct an atomically dispersed MoS2.Co catalyst with modulated local electronic structure, definite chemical environment and enhanced oxygen evolution reaction performance. Theoretical calculations indicate that immsobilized single-Co sites exhibit an optimized adsorption capability of oxygencontaining intermediates, endowing the catalyst an excellent electrocatalytic oxygen evolution reaction activity, with a low overpotential of 370 mV at10 mA cm-2.nd a small Tafel slope of 90 mV dec-1. The extendable potential of this strategy to other electrocatalysts such as MoS2.Ni and MoS2.Zn, and other applications such as the hydrogen evolution reaction was also demonstrated. This study affords new insights into the rational design of single metal atom systems with enhanced electrocatalytic performance.

关键词： electrocatalysis oxygen evolution reaction pillararenequinone single atoms transition-metal dichalcogenides

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Graphdiyne(C_(n)H_(2.-2.)as an"electron transfer bridge"boosting photocatalytic hydrogen evolution over Zn_(0.5)Co_(0.5)S/MoS_(2.S-scheme heterojunction

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Rare Metals 2024年第5期43卷 1999-2014页

作者： Mei Li Jing-Zhi Wang Zhi-Liang Jin School of chemistry and chemical {2. North Minzu UniversityYinchuan 750021China School of chemistry and chemical {2. Ningxia Key Laboratory of Solar Chemical Conversion TechnologyKey Laboratory for Chemical Engineering and TechnologyState Ethnic Affairs CommissionNorth Minzu UniversityYinchuan 750021China

In the process of photocatalytic water cracking,the migration rate and utilization rate of photogenerated charges determine the hydrogen evolution performance of the *** this paper,a carbon isotope superconducting material graphdiyne(GDY)is prepared by mechanical ball milling and introduced into the S-scheme heterojunction Zn_(0.5)Co_(0.5)S/MoS_(2.inorganic *** terms of hydrogen evolution kinetics,GDY acts as an electron bridge,not only accelerating the migration of photogenerated carriers but also improving the utilization of photogenerated ***,the large twodimensional layer provides more loading and anchoring points for Zn_(0.5)Co_(0.5)S/MoS_(2.,which increases the number of active *** ternary composite catalyst 2.%GDY/Zn_(0.5)Co_(0.5)S/MoS_(2.(2.-GCSM)generates 69.94μmol of hydrogen(5 h)in triethanolamine *** is 2.97 and1.80 times higher than Zn_(0.5)Co_(0.5)S and Zn_(0.5)Co_(0.5)S/MoS_(2.,*** the cyclic experiment,it still has stable hydrogen evolution performance after standing for2. h(under dark conditions).In addition,the potential mechanism of photocatalytic hydrogen evolution is demonstrated through in-situ X-ray photoelectron *** work provides a reference for further research in the field of introducing carbon materials into photocatalytic systems and improving the utilization of photogenerated charges.

关键词： Graphdiyne S-scheme heterojunction Electron transfer bridge Hydrogen production

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S-scheme heterojunction in photocatalytic hydrogen production

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Journal of Materials Science & Technology 2024年第2期169卷 82-104页

作者： Teng Li Noritatsu Tsubaki Zhiliang Jin School of chemistry and chemical {2. North Minzu UniversityYinchuan 750021China department of Applied chemistry Graduate School of EngineeringUniversity of ToyamaGofuku 3190Toyama 930-8555Japan

As an ideal secondary energy source,hydrogen has the title of clean energy and the product of its complete combustion is only water,which is not polluting to the *** hydrogen production technology is an environmentally friendly,safe,and low-cost strategy that requires only an inexhaustible amount of solar energy and water as *** paper provides a detailed and detailed review of S-scheme heterojunction photocatalysts for photocatalytic hydrogen production,mainly including TiO_(2.-based,Perovskite-based,CdS-based,Graphitic phase carbon nitride-based,COF-based graphdiyne-based,ZnO-based,and ZnIn_(2.S_(4)-based S-scheme heterojunction *** classification of S-scheme heterojunctions is ***’s more,various characterizations for direct verification of the charge migration mechanism of S-scheme heterojunctions are *** on the present study,the future potential challenges and future research trends for S-scheme heterojunctions in photocatalytic hydrogen evolution technology are pointed out,which provides feasible strategies for the development and design of S-scheme heterojunction photocatalysts in the field of photocatalytic hydrogen evolution.

关键词： S-scheme heterojunction Photocatalysis Charges migration Hydrogen evolution

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Coupling Co2. nanoparticles onto N,P-doped biomass-derived carbon as efficient electrocatalysts for flexible Zn–air batteries

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Rare Metals 2024年第10期43卷 4982-4991页

作者： Shu-Qi Li Kang Sun Yan-Yan Liu Shu-Ling Liu Jing-Jing Zhou Wen-Bo Zhang Yi-Hang Lu Xiang-Meng Chen Xiao-Peng Wang Bao-Jun Li Jian-Chun Jiang College of Science Henan Agricultural University department of chemistry Tsinghua University College of chemistry Zhengzhou University Institute of chemical Industry of Forest Products National Engineering Lab for Biomass Chemical UtilizationKey and Open Lab on Forest Chemical EngineeringChinese Academy of ForestryState Forestry Administration

Catalysts for oxygen conversion play an important role in energy storage and conversion technologies such as metal-air *** highly active stable,and low-cost catalysts is critical for further implementation of the above ***,an efficien oxygen electrocatalyst with Co2. nanoparticles （NPs）coupling onto N,P-doped porous carbon nanosheets（Co2.@NPAC） derived from cotton stalk is successfully designed and prepared via activation,hydrothermal treatment,and pyrolysis *** excellent properties of electrical conductivity,mass transfer,and synergistic integration between Co2. and N,P-doped carbon endow Co2.@NPAC composite with superior oxygen reduction reaction/oxygen evolution reaction （ORR/OER） ***2.@NPAC catalyst achieves ORR activity with half-wave potential of 0.85 V and high OER activity with overpotential of 2.1 mV at 10 mA·*** flexible Zn-air batteries （ZABs） based on Co2.@NPAC catalyst revea outstanding performances with a high open-circuit voltage（1.38 V）,a peak power density of (75 mW·cm-2.,and a low charge-discharge voltage gap （0.74 V,～2.0 cycles）The flexible ZABs express the stable discharge-charge voltage gap at various bending *** work provides interesting inspiration for the ingenious design of efficien carbon electrocatalysts from biomass with potential application of energy storage and conversion devices.

关键词： Cotton stalk Flexible Zn–air batteries N,P-doped activated carbon Oxygen reduction reaction

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Micro-nano-fabrication of green functional materials by multiphase microfluidics for environmental and energy applications

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Green Energy & Environment 2024年第8期9卷 1199-1219页

作者： Cheng Qi Tao Zhou Xingjiang Wu Kailang Liu Lei Li Zhou Liu Zhuo Chen Jianhong Xu Tiantian Kong Guangdong Provincial Key Laboratory of Micro/Nano Optomechatronics engineering College of Mechatronics and Control EngineeringShenzhen University The State Key Laboratory of chemical engineering Department of Chemical EngineeringTsinghua University College of chemistry and Environmental engineering Shenzhen University department of Biomedical engineering School of MedicineShenzhen University

Multiphase microfluidic has emerged as a powerful platform to produce novel materials with tailor-designed functionalities, as microfluidic fabrication provides precise controls over the size, component, and structure of resultant materials. Recently, functional materials with welldefined micro-/nanostructures fabricated by microfluidics find important applications as environmental and energy materials. This review first illustrated in detail how different structures or shapes of droplet and jet templates are formed by typical configurations of microfluidic channel networks and multiphase flow systems. Subsequently, recent progresses on several representative energy and environmental applications, such as water purification, water collecting and energy storage, were overviewed. Finally, it is envisioned that integrating microfluidics and other novel materials will play increasing important role in contributing environmental remediation and energy storage in near future.

关键词： Microfluidics Multi-phase flow Droplet and microfiber Environmental remediation Energy Storage

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Multiple interface coupling on natural tourmaline enables high-efficiency removal of antibiotic:Superior property and mechanism

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Journal of Environmental Sciences 2024年第6期140卷 242-254页

作者： Jingjing Cui Xiangyu Liu Feifan Qie Chengzhe Xie Qingdong He Jian Liu Steven L.Suib Wenbo Wang College of chemistry and chemical {2. Inner Mongolia UniversityHohhot 010021China department of chemistry University of ConnecticutStorrsCT 06269-3060United States

Reasonably designing highly active,environmentally friendly,and cost-effective catalysts for efficient elimination of pollutants from water is desirable but ***,an efficient heterogeneous photo-Fenton catalyst tourmaline(TM)/tungsten oxide(WO_(3-x))(named TW10)containing tungsten/boron/iron(W/B/Fe)synergistic active centers and 90%of cheap natural tourmaline(TM)mineral rich in Fe and B *** TW10 catalyst can quickly activate peroxymonosulfate(PMS)to generate massive active free radicals,which may induce the rapid and efficient degradation of tetracycline(TC).The TW10/PMS/Visible light system can effectively degrade up to 98.7%of tetracycline(TC)in actual waters(***,Yellow River,and Yangtze River water),and the catalytic degradation rates reach 1.65,5.569,and 2.38 times higher than those of TM,WO_(3-x),and commercial P2.(Degussa,Germany),*** addition,the catalyst can be recycled and reused multiple *** spin resonance spectroscopy(EPR),X-ray photoelectron spectroscopy(XPS),and liquid chromatograph-mass spectrometer(LC-MS)analyses confirm that the synergistic catalytic effect of W/B/Fe sites on the TW10 catalyst accelerates the electron transfer between Fe(Ⅱ)and Fe(Ⅲ),as well as between W(Ⅴ)and W(Ⅵ),and thus promotes the rapid degradation of *** catalytic reaction mechanism and degradation pathway of TC were *** work provides a feasible route for the design and development of new eco-friendly and efficient catalyst.

关键词： Tourmaline(TM) Fenton-like catalyst Tungsten oxide Peroxymonosulfate Antibiotic

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