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Hierarchical cobalt-molybdenum layered double hydroxide arrays power efficient oxygen evolution reaction

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Nano Research 2024年第6期17卷 5080-5086页

作者： Xinyi Zhu Jiahui Lyu Shanshan Wang Xingchuan Li Xiaoyu Wei Cheng Chen Wanida Kooamornpattana Francis Verpoort Jinsong Wu zongkui kou State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070China Sanya Science and Education Innovation Park of Wuhan University of Technology Sanya 572000China Nanostructure Research Center Wuhan University of TechnologyWuhan 430070China Department of Chemical Engineering Faculty of EngineeringMahidol UniversityNakhon Pathom 73170Thailand

Transition metal-based layered double hydroxides(LDHs)have been capable of working efficiently as catalysts in the basic oxygen evolution reaction(OER)for sustaining hydrogen production of alkaline water ***,exploring new LDH-based electrocatalysts featuring both remarkable activity and good stability is still in high demand,which is pivotal for comprehensive understanding and impressive improvement of the sluggish OER ***,a series of bimetallic(Co and Mo)LDH arrays were designed and fabricated via a facile and controlled strategy by incorporating a Mo source into presynthesized Co-based metal-organic framework(MOF)arrays on carbon cloth(CC),named as ZIF-67/CC *** found that tuning the Mo content resulted in gradual differences in the structural properties,surface morphology,and chemical states of the resulting catalysts,namely CoMox-LDH/CC(x representing the added weight of the Mo source).Gratifyingly,the best-performing CoMo_(0.20)-LDH/CC electrocatalyst demonstrates a low overpotential of only 226 mV and high stability at a current density of 10 mA·cm^(−2),which is superior to most LDH-based OER catalysts reported ***,it only required 1.611 V voltage to drive the overall water splitting device at the current density of 10 mA·cm^(−2).The present study represents a significant advancement in the development and applications of new OER catalysts.

关键词： layered double hydroxides(LDHs) metal-organic frameworks(MOFs) array catalysts Mo modification electrocatalytic oxygen evolution reaction(OER)

Single‑Atom Catalysts:Advances and Challenges in Metal‑Support Interactions for Enhanced Electrocatalysis

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Electrochemical Energy Reviews 2022年第1期5卷 145-186页

作者： Yang Mu Tingting Wang Jian Zhang Changgong Meng Yifu Zhang zongkui kou School of Chemical Engineering Dalian University of TechnologyDalian 116024LiaoningChina State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070HubeiChina School of Chemistry and Chemical Engineering Huazhong University of Science and TechnologyWuhan 430074HubeiChina

Single-atom catalysts(SACs),which contain a single metal atom supported on a well-confined substrate,are among the most promising heterogeneous catalysts owing to their unique advantages,such as high intrinsic activity and selectivity,tunable bonds and coordination,abundant metal-containing active sites,and atomic *** metal-support interactions(MSIs)in SACs exert a substantial influence on the catalytic properties,gaining a profound understanding and recognition of catalytic reactions depends greatly on investigating MSIs both experimentally and ***,the engineer-ing and modulation of MSIs are regarded as one of the most efficient methods to rationally design SACs with disruptively enhanced catalytic *** this review,we track the recent advances in SACs from an MSI *** then discuss the existing MSIs in SACs and elucidate the significant role of strong MSIs in catalytic properties and *** chal-lenges hindering the rational design of supported SACs with strong MSIs,which are currently still far from being completely understood and overcome,are *** addition,the correlation between strong MSIs and electrocatalytic activities in SACs,including an outlook to increase our understanding of MSIs,is ***,the present review provides some perspectives and an in-depth understanding of strong MSIs to advance high-performing SACs.

关键词： Metal-support interaction Single-atom catalysts Electrocatalysis ORR and OER HER and HOR

Fundamentals,On‑Going Advances and Challenges of Electrochemical Carbon Dioxide Reduction

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Electrochemical Energy Reviews 2022年第1期5卷 82-111页

作者： zongkui kou Xin Li Tingting Wang Yuanyuan Ma Wenjie Zang Guangdi Nie John Wang Department of Materials Science and Engineering National University of SingaporeSingapore 117574Singapore Shenzhen Engineering Laboratory of Phosphorene and Optoelectronics International Collaborative Laboratory of 2D Materials for Optoelectronics Science and TechnologyCollege of Physics and Optoelectronic EngineeringShenzhen UniversityShenzhen 518060GuangdongChina Industrial Research Institute of Nonwovens and Technical Textiles College of Textiles and ClothingQingdao UniversityQingdao 266071ShandongChina

Electrochemical carbon dioxide reduction(ECR)is an attractive pathway to synthesize useful fuels and chemical feedstocks,especially when paired with renewable electricity as the energy *** this overview,we examine the recently witnessed advances and on-going pursuits of ECR in terms of the key fundamental mechanisms,basic experimentation principles,electrocatalysts and the electrochemical setup for ECR,aiming at offering timely key insights into solving the unsettled bottleneck *** reaction pathways are discussed in relation to the generation of single-,double-and multi-carbon products by the ECR,as well as the underlying principles in catalyst design to form them both efficiently and *** the rational design of electrocatalysis,we look into the critically important roles played by various in situ and operando experimental techniques and computational simulations,where the key priorities are to engineer the highly active and selec-tive ECR catalysts for the specifically targeted ***,with the purposely designed high activity and selectivity,one would be able to“magically”transform a bottle of CO_(2)-riched“coke drink”to a glass of“beer”with the desired alcohol product in a layman term,instead of a bottle of formic ***,there are still considerable complications and challenges *** a dynamically rapid-advancing research frontier for both energy and the environment,there are great opportunities and obstacles in the ECR scale up.

关键词： CO_(2)reduction Electrocatalysis Catalyst design Mechanism understanding Fundamental science

Constructing a stable cobalt-nitrogen-carbon air cathode from coordinatively unsaturated zeolitic-imidazole frameworks for rechargeable zinc-air batteries

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Nano Research 2022年第7期15卷 5895-5901页

作者： Tingting Wang Meng Liu Somboon Chaemchuen Jichao Wang Ye Yuan Cheng Chen Ang Qiao Francis Verpoort zongkui kou State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070China

Zeolitic-imidazole frameworks(ZIFs)derivations have widely emerged as an efficient air cathode of zinc-air batteries(ZABs)due to excellent bifunctional oxygen electrocatalysis ***,they are not stable enough for long-term operation of rechargeable ZABs because of weak association with current collector,especially under bending conditions for flexible ZAB ***,we show that by purposely designing coordinatively unsaturated ZIFs via a facile morphology regulation,which can be chemically linked on acid-treated carbon cloth,a stable Co-N-C air cathode is therefore derived where Co nanoparticles(NPs)are uniformly confined within the Co-N-C matrix on carbon cloth(Co/Co-N-C/CC).Specifically,when without being stabilized from carbon cloth,the pyrolysis of ZIFs with different unsaturated coordination levels has a negligible impact on the bifunctional oxygen-catalyzed *** optimal Co/Co-N-C/CC catalyst assembled ZAB possesses a large open circuit voltage of 1.415 V and a high peak power density of 163 mW·cm^(−2) as well as excellent cycling durability upon 630 discharge–charge cycles with 61%voltage efficiency remained,largely exceeding those of a benchmark Pt/C-IrO_(2) catalyst assembled *** synergy between Co NPs and active Co-N-C sites via electronic interaction induces the outstanding bifunctional oxygen-catalyzed activity and cathode *** present work highlights the importance of unsaturated coordination structures in ZIFs precursors for the performance of derived nanostructures in integrated electrodes.

关键词： coordinatively unsaturated zeolitic-imidazole frameworks(ZIFs) cobalt-nitrogen-carbon bifunctional air electrodes zincair battery flexible electrode

Vertically mounting molybdenum disulfide nanosheets on dimolybdenum carbide nanomeshes enables efficient hydrogen evolution

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Nano Research 2022年第5期15卷 3946-3951页

作者： Tingting Wang Pengyan Wang Yajun Pang Yitian Wu Jin Yang Hao Chen Xiaorui Gao Shichun Mu zongkui kou State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070China College of Chemistry and Materials Engineering Zhejiang A&F UniversityHangzhou 311300China Jiangsu Laboratory of Advanced Functional Materials School of Electronic and Information EngineeringChangshu Institute of TechnologyChangshu 215500China

Designing hierarchical heterostructure to optimize the adsorption of hydrogen intermediate(H*)is impressive for hydrogen evolution reaction(HER)***,we show that vertically mounting two-dimensional(2D)layered molybdenum disulfide(MoS_(2))nanosheets on 2D nonlayered dimolybdenum carbide(Mo_(2)C)nanomeshes to form a hierarchical heterostructure largely accelerates the HER kinetics in acidic electrolyte due to the weakening adsorption strength of H*on 2D Mo_(2)C *** hierarchical MoS2/Mo2C heterostructure therefore gives a decrease of overpotential for up to 500 mV at-10 mA·cm^(-2)and an almost 200-fold higher kinetics current density compared with the pristine Mo2C nanomeshes and maintains robust stability with a small drop of overpotential for only 16 mV upon 5,000 *** further rationalize this finding by theoretical calculations and find an optimized adsorption free energy of H*,identifying that the MoS_(2)featuring strong H*desorption plays a key role in weakening the strong binding of Mo_(2)C with H*and therefore improves the intrinsic HER activity on active C sites of Mo_(2)*** present finding shines the light on the rational design of heterostructured catalysts with synergistic geometry.

关键词： hydrogen evolution reaction transition metal carbide transition metal disulfide two-dimensional nonlayered/layered heterostructure hydrogen adsorption/desorption

In situ confined vertical growth of Co_(2.5)Ni_(0.5)Si_(2)O_(5)(OH)_(4)nanoarrays on rGO for an efficient oxygen evolution reaction

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Nano Materials Science 2023年第4期5卷 351-360页

作者： Yang Mu Xiaoyu Pei Yunfeng Zhao Xueying Dong zongkui kou Miao Cui Changgong Meng Yifu Zhang State Key Laboratory of Fine Chemicals School of Chemical EngineeringDalian University of TechnologyDalian116024China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan430070China

Rational design of oxygen evolution reaction(OER)catalysts at low cost would greatly benefit the *** advantage of earth-abundant elements Si,Co and Ni,we produce a unique-structure where cobalt-nickel silicate hydroxide[Co_(2.5)Ni_(0.5)Si_(2)O_(5)(OH)_(4)]is vertically grown on a reduced graphene oxide(rGO)support(CNS@rGO).This is developed as a low-cost and prospective OER *** to cobalt or nickel silicate hydroxide@rGO(CS@rGO and NS@rGO,respectively)nanoarrays,the bimetal CNS@rGO nanoarray exhibits impressive OER performance with an overpotential of 307 mV@10 mA cm^(-2).This value is higher than that of CS@rGO and NS@*** CNS@rGO nanoarray has an overpotential of 446 mV@100 mA cm^(-2),about 1.4 times that of the commercial RuO_(2)*** achieved OER activity is superior to the state-of-the-art metal oxides/hydroxides and their *** vertically grown nanostructure and optimized metal-support electronic interactions play an indispensable role for OER performance improvement,including a fast electron transfer pathway,short proton/electron diffusion distance,more active metal centers,as well as optimized dualatomic electron *** advantage of interlay chemical regulation and the in-situ growth method,the advanced-structural CNS@rGO nanoarrays provide a new horizon to the rational and flexible design of efficient and promising OER electrocatalysts.

关键词： Co_(2.5)Ni_(0.5)Si_(2)O_(5)(OH)_(4)@rGO Vertical grown nanoarrays Geometric and electronic structure regulation Metal-support interactions Oxygen evolution reaction

Well-structured 3D channels within GO-based membranes enable ultrafast wastewater treatment

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Nano Research 2023年第2期16卷 1826-1834页

作者： Huaqiang Fu Zhe Wang Peng Li Wei Qian Zixin Zhang Xin Zhao Hao Feng Zhugen Yang zongkui kou Daping He School of Materials Science and Engineering Wuhan University of TechnologyWuhan 430070China Hubei Engineering Research Center of RF-Microwave Technology and Application School of ScienceWuhan University of TechnologyWuhan 430070China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070China School of Water Energy and EnvironmentCranfield UniversityCranfield MK430ALUK

Graphene oxide(GO)-based membranes have been widely studied for realizing efficient wastewater treatment,due to their easily functionalizeable surfaces and tunable interlayer ***,the irregular structure of water channels within GO-based membrane has largely confined water permeance and prevented the simultaneously improvement of purification ***,we purposely construct the well-structured three-dimensional(3D)water channels featuring regular and negatively-charged properties in the GO/SiO_(2)composite membrane via in situ close-packing assembly of SiO_(2)nanoparticles onto GO *** regular 3D channels can improve the water permeance to a record-high value of 33,431.5±559.9 L·m^(−2)·h−1(LMH)bar−1,which is several-fold higher than those of current state-of-the-art GO-based *** further demonstrate that benefiting from negative charges on both GO and SiO2,these negatively-charged 3D channels enable the charge selectivity well toward dye in wastewater where the rejection for positive-charged and negative-charged dye molecules is 99.6%vs.7.2%,*** 3D channels can also accelerate oil/water(O/W)separation process,in which the O/W permeance and oil rejection can reach 19,589.2±1,189.7 LMH bar−1 and 98.2%,*** present work unveils the positive role of well-structured 3D channels on synchronizing the remarkable improvement of both water permeance and purification performance for highly efficient wastewater treatment.

关键词： graphene oxide membranes wastewater treatment water channels charge-selectivity

Single-atom metal-nitrogen-carbon catalysts energize single molecule detection for biosensing

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InfoMat 2023年第6期5卷 44-65页

作者： Xianyang Zhang Pengfei Chen Siwuxie He Bowen Jiang Yong Wang Yonghua Cheng Jian Peng Francis Verpoort John Wang zongkui kou State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhanthe People's Republic of China “ZhuCai”Center of Innovation and Entrepreneurship Wuhan University of TechnologyWuhanthe People's Republic of China West China School of Pharmacy Sichuan UniversityChengduthe People's Republic of China Department of Materials Science and Engineering Faculty of EngineeringNational University of SingaporeSingapore Institute of Materials Research and Engineering A*StarSingapore

Biosensors featuring single molecule detection present huge opportunities as well as challenges in food safety inspection,disease diagnosis,and environmental ***-molecule detection is largely lacking of high enough activity,precision molecule selectivity,and understanding in the exact operating ***-atom catalysts(SACs),especially those metals-nitrogen-carbon that mimic the natural metalloenzyme structure,and with well-defined metal atom bond configurations,high level of molecular selectivity,and easy fabrication,endow single molecule detections with practical-use *** recent advances in single-atom catalysts also present new pathways in the key mechanism *** this short review,we will first visit the brief history and advantages of SACs that have been explored only recently for molecule-scale biosensors,where they are analogous and also differentiated from those nanozymes and natural *** applications in electrochemical,photochemical,and photoelectrochemical sensors are then discussed comprehensively by focusing on the different molecule-scale sensing modes in achieving local coordination-modulated signal ***,we identify new opportunities and challenges faced by these SACs-based single molecule detections in the further development of biosensors.

关键词： biosensors metal-nitrogen-carbon nanozyme single molecule detection single-atom catalysts

Nurturing the marriages of single atoms with atomic clusters and nanoparticles for better heterogeneous electrocatalysis

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Interdisciplinary Materials 2022年第1期1卷 51-87页

作者： Lei Zhang Jiawei Zhu Xin Li Shichun Mu Francis Verpoort Junmin Xue zongkui kou John Wang Department of Materials Science and Engineering National University of SingaporeSingaporeSingapore State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhanChina School of Physical&Mathematical Sciences Nanyang Technological UniversitySingaporeSingapore

Single-atom catalysts,featuring some of the most unique activities,selectivity,and high metal utilization,have been extensively studied over the past *** their high activity,selectivity,especially towards small molecules or key intermediate conversions,they can be synergized together with other active species(typically other single atoms,atomic clusters,or nanoparticles)in either tandem or parallel or both,leading to much better performance in complex catalytic *** there have been reports on effectively combining the multiple components into one single catalytic entity,the combination and synergy between single atoms and other active species have not been reviewed and examined in a systematic ***,in this overview,the key synergistic interactions,binary complementary effects,and the bifunctional functions of single atoms with other active species are defined and discussed in *** integration functions of their marriages are in-vestigated with particular emphasis on the homogeneous and heterogeneous combinations,spatial distribution,synthetic strategies,and the thus-derived outstanding catalytic performance,together with new light shined on the catalytic mechanisms by zooming in several case *** dynamic nature of each of the active species and in particular their interactions in such new catalytic entities in the heterogeneous electrocatalytic processes are visited,on the basis of the in situ/operando ***,we feature the current chal-lenges and future perspectives of these integrated catalytic entities that can offer guidance for advanced catalyst design by the rational combination and synergy of binary or multiple active species.

关键词： atomic clusters binary/multiple synergy heterogeneous catalysis nanoparticles single atoms