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Atomically precise nickel-sulfur clusters for efficient electrochemical 2,5-hydroxymethylfurfural oxidation

Nano Research 2025年第1期18卷 140-148页

作者： Fen Wang Lu-Yu Liu Sha-Sha Cui Ting-Ting Li Xiao-Meng Yang Zhijuan Liu Yanyong Wang Henan key laboratory of Crystalline Molecular Functional Materials Henan International Joint Laboratory of Tumor Theranostical Cluster MaterialsGreen Catalysis Centerand College of ChemistryZhengzhou UniversityZhengzhou 450001China State key laboratory of chem/bio-sensing and chemometrics College of Chemistry and Chemical EngineeringHunan UniversityChangsha 410082China

Nickel sulfide exhibits excellent catalytic activity in the electrochemical 2,5-hydroxymethylfurfural oxidation reaction(HMFOR).However,due to the polydispersity of nanoparticles,it is difficult to establish a clear structure-activity relationship at the atomic *** this work,we have successfully synthesized atomically precise Ni_(6)(PET)_(12)and Ni_(4)(PET)_(8)clusters(PET:2-phenylethanethiol)for ***^(2+)and S_(2)-with atomic ratio of 1:2 was mainly existed in Ni_(6)(PET)_(12)and Ni_(4)(PET)_(8)to form Ni-S *** electrochemical test results have suggested both Ni_(6)(PET)_(12)and Ni_(4)(PET)_(8)displayed outstanding electrocatalytic ability for *** Ni_(6)(PET)_(12)exhibited better electrocatalytic ability than Ni_(4)(PET)_(8)with higher current density,lower overpotential and faster reaction *** superior electrochemical ability of Ni_(6)(PET)_(12)may be due to the enhanced adsorption towards HMF molecule with strong interaction towards hydroxyl group and furan ***,it found that the Ni^(2+)species in Ni_(6)(PET)_(12)could rapidly oxidized into Ni^(3+)species,which could spontaneously capture electron and proton from HMF for *** theoretical calculation demonstrated that the Ni_(6)(PET)_(12)process lower free energy barrier than Ni_(4)(PET)_(8)to display excellent electrocatalytic *** work is of great significance for designing efficient electrocatalysts for HMFOR.

关键词： atomically precise nickel nanoclusters 2 5-hydroxymethylfurfural electro-oxidation Ni3+species

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Transforming Co3O4 nanosheets into porous N-doped CoxOy nanosheets with oxygen vacancies for the oxygen evolution reaction

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Journal of Energy chemistry 2019年第8期28卷 24-29,I0002页

作者： Lei Xu Yuqin Zou Zhaohui Xiao Shuangyin Wang State key laboratory of chem/bio-sensing and chemometrics College of Chemistry and Chemical Engineering Hunan University

Cobalt oxides have been widely investigated as promising replacements for noble metal-based catalysts for oxygen evolution reaction(OER). Herein, we, for the first time, have obtained porous CoxOy nanosheets with N-doping and oxygen vacancies by etching Co3O4 nanosheets with NH3 plasma. Comparing with the pristine Co3O4 nanosheets(1.79 V), the porous CoxOy nanosheets with N-doping and oxygen vacancies have a much lower potential of 1.51 V versus RHE to reach the current density of 10 mA cm-2. The obtained sample has a lower Tafel slope of 68 m V dec-1 than the pristine Co3O4 nanosheets(234 mV dec-1).The disclosed Co^2+, which is responsible for the formation of active sites(CoOOH), N-doping and oxygen vacancies, gives rise to better performance of OER.

关键词： Electrocatalysts Oxygen evolution reaction Cobalt oxides N doping Oxygen vacancies

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Recent advances in defect electrocatalysts: Preparation and characterization

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Journal of Energy chemistry 2021年第2期30卷 208-225,I0008页

作者： Zhaohui Xiao Chao Xie Yanyong Wang Ru Chen Shuangyin Wang State key laboratory of chem/bio-sensing and chemometrics College of Chemistry and Chemical EngineeringHunan UniversityChangsha 410082HunanChina

the types and strategies used to prepare defect electrocatalysts will continue to be studied and developed as new defective materials are generated.4. Characterization of defectsThis review briefly summarizes recent progress in defect electrocatalysts, and the synthesis strategies and characterization techniques for defects are systematically discussed. Although challenges in the characterization of defect structures in the electrocatalytic reaction process remain, the dynamic evolution of defect sites is predicted to be helpful for designing and preparing high-performance electrocatalysts for commercial applications. Furthermore, due to an insufficient understanding of the defect-structureproperty relationships, future possibilities for the reasonable design of defect electrocatalysts to obtain desirable performance are suggested.

关键词： Defect Electrocatalysts Vacancies Heteroatom doping

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An option for green and sustainable future: Electrochemical conversion of ammonia into nitrogen

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Journal of Energy chemistry 2021年第9期30卷 384-402页

作者： Bo Zhou Nana Zhang Yujie Wu Weijun Yang Yanbing Lu Yanyong Wang Shuangyin Wang State key laboratory of chem/bio-sensing and chemometrics College of Chemistry and Chemical EngineeringHunan UniversityChangsha 410082HunanChina

Green and sustainable options are needed to ease the current energy and environmental crisis, and alleviate the greenhouse effect and energy shortage. As an alternative carbon–neutral synthetic fuel, ammonia shows great potential due to its high energy density, non-toxic by-products, and mature related infrastructures. However, related practical applications have been severely hampered on ammoniaoxidation due to the high cost of catalysts and immature energy utilization systems. Here, we comprehensively summarized the efforts which have been made in recent years with the aim of providing a deep sight into the development and deficiencies in this territory and trying to establish a simple framework of basic knowledge for researchers. The exploration of mechanism is discussed first and then the relevant catalysts studied in recent years are summarized. Besides, the progress of direct ammonia fuel cells(DAFCs) is also presented and the challenges as well as perspectives on future developments of electrocatalysts for ammonia electro-oxidation and its practical application are provided at the end.

关键词： Ammonia Ammonia electro-oxidation reaction(AOR) Mechanism Electrocatalysts DAFCs

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Three-dimensional hierarchical MoS_2/CoS_2 heterostructure arrays for highly efficient electrocatalytic hydrogen evolution

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Green Energy & Environment 2017年第2期2卷 134-141页

作者： Canbin Ouyang Shi Feng Jia Huo Shuangyin Wang State key laboratory of chem/bio-sensing and chemometrics Provincial Hunan Key Laboratory for Graphene Materials and Devices College of Chemistry and Chemical Engineering Hunan University

Developing non-expensive, highly active and highly stable electrocatalysts for hydrogen evolution has aroused extensive attention, owing to the necessity of novel clean and sustainable energy carriers. In this paper, we report a synthesis of free-standing three-dimensional hierarchical MoS_2/CoS_2 heterostructure arrays through a convenient process. The investigation of electrocatalytic HER performance suggests that the MoS_2/CoS_2 hybrid catalyst exhibits significant enhancement in HER(onsetpotential and potential at a current density of 100 mA cm^(-2) are 20 mV and125 mV, respectively) and superior durability(no shift of current density is observed after a continuous scanning of 3000 times) compared with individual CoS_2 and MoS_2. The superior HER performance was attributed to the formation of the interface between CoS_2 and MoS_2 through the electrochemical characterization, Raman, XPS analysis, and the control experiment. The lower onsetpotential, higher current density, excellent durability, and the free-standing structure of the three-dimensional hierarchical MoS_2/CoS_2 heterostructure array make it a promising cathode catalyst suitable for widespread application.

关键词： MoS2/CoS2 Heterostructure array Free-standing Hydrogen evolution reaction

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Rational design of three-phase interfaces for electrocatalysis

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Nano Research 2019年第9期12卷 2055-2066页

作者： Yuqing Wang Yuqin Zou Li Tao Yanyong Wang Gen Huang Shiqian Du Shuangyin Wang State key laboratory of chem/bio-sensing and chemometrics Provincial Hunan Key Laboratory for Graphene Materials and De vicesCollege oj Chemistry and Chemical EngineeringHunan UniversityChangsha 410082China

Gas-involving electrochemical reactions,like oxygen reduction reaction (ORR),oxygen evolution reaction (OER),and hydrogen evolution reaction (HER),are critical processes for energy-saving,environment-friendly energy conversion and storage technologies which gain increasing *** development of according electrocatalysts is key to boost their electrocatalytic *** efforts have been put into the development of advanced electrocatalysts to overcome sluggish *** the other hand,the electrode interfaces-architecture construction plays an equally important role for practical applications because these imperative electrode reactions generally proceed at triple-phase interfaces of gas,liquid electrolyte,and solid electrocatalyst.A desirable architecture should facilitate the complicate reactions occur at the triple-phase interfaces,which including mass diffusion,surface reaction and electron *** this review,we will summarize some design principles and synthetic strategies for optimizing triple-phase interfaces of gas-involving electrocatalysis systematically,based on the electrode reaction process at the three-phase *** can be divided into three main optimization directions:exposure of active sites,promotion of mass diffusion and acceleration of electron ***,we especially highlight several remarkable works with comprehensive optimization about specific energy conversion devices,including metal-air batteries,fuel cells,and water-splitting devices are demonstrated with superb *** the last section,the perspectives and challenges in the future are proposed.

关键词： triple-phase irderfaces gas-involving electrocatalysis mass diffusion exposure of active sites electron transfer

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LDHs derived nanoparticle-stacked metal nitride as interlayer for long-life lithium sulfur batteries

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Science Bulletin 2018年第3期63卷 169-175页

作者： Zhen Li Zhaoling Ma Yanyong Wang Ru Chen Zhenjun Wu Shuangyin Wang State key laboratory of chem/bio-sensing and chemometrics Provincial Hunan Key Laboratory for Graphene Materials and Devices College of Chemistry and Chemical Engineering Hunan University key laboratory of Optoelectronic Devices and Systems of Ministry of Education and Guangdong Province Shenzhen University

Shuttle effect is one of the most serious disadvantages in lithium-sulfur battery which results in poor cycle performance and hinders the commercialization of Li-S *** reduce the dissolution of polysulfides into the electrolyte and prolong the cycling stability,nanoparticle-stacked metal nitride derived from layered double hydroxides(LDHs)as an interlayer was inserted between sulfur cathode and separator to confine polysulfides by physical and chemical ***,the surface of metal nitride will form an oxide passivation *** passivation layer possesses hydrophilic metal-O group and provides a polar surface for strong binding with ***’s more,the nanoparticlesstacked structure could immerge and retain electrolyte well,which could enhance the ability of promoting the electron exchange *** sulfur electrode with nanoparticle-stacked metal nitride interlayer has an excellent cycle performance owing to the interactions between metal nitride and *** battery delivered an initial capacity of 764.6 m Ahg^(-1) and still possesses a capacity of 477.5 mAhg^(-1) with the retention of 62.4% after 800 cycles.

关键词： Nanoparticle-stacked structure Metal nitride InterlayerLithium polysulfides Li-S batteries

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Liquid Metal-Based Self-Healable and Elastic Conductive Fiber in Complex Operating Conditions

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Energy & Environmental Materials 2023年第6期6卷 297-304页

作者： Yin Zhou Yingying Zhu Zuan Hu Xiaoying Yang Pengkun Yang Lu Huang Yingpeng Wu State key laboratory of chem/bio-sensing and chemometrics Advanced Catalytic Engineering Research Center of the Ministry of EducationCollege of Chemistry and Chemical EngineeringHunan UniversityChangsha 410082China

Flexible conductive fibers are essential for wearable electronics and smart electronic ***,in complex operating conditions,conductive fibers will inevitably fracture or ***,we have developed an elastic conductive self-healable fiber(C-SHF),of which the electrical and mechanical properties can efficiently heal in a wide operating range,including room temperature,underwater,and low *** advantage can be owed to the combination of reversible covalent imine bond and disulfide bond,as well as the instantaneous self-healing ability of liquid *** C-SHF,with stretchability,conductivity stability,and universal self-healing properties,can be used as an electrical signal transmission line at high strain and under different operating ***,C-SHF was assembled into a double-layer capacitor structure to construct a self-healable sensor,which can effectively respond to pressure as a wearable motion detector.

关键词： complex operating conditions elastic conductive fiber liquid metal self-healing

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Recent Progress on Electrocatalytic Valorization of biomass-Derived Organics

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Energy & Environmental Materials 2022年第4期5卷 1117-1138页

作者： Ming Yang Zhenran Yuan Rixin Peng Shuangyin Wang Yuqin Zou State key laboratory of chem/bio-sensing and chemometrics Provincial Hunan Key Laboratory for Graphene Materials and DevicesCollege of Chemistry and Chemical EngineeringHunan UniversityChangsha 410082China E-mail:yuqin_zou@***

Electrocatalytic valorization of biomass derivatives can be powered by electricity generated from renewable sources such as solar and wind energy.A shift from centralized,high-temperature,and energy-intensive processes to decentralized,low-temperature conversions is achieved,which meets the requirement of sustainable energy *** approach provides an efficient,green,and additive-free strategy for biomass derivative valorization,in which product selectivity could be easily regulated by the applied potential and electrocatalyst ***,a scale-up application is still far from being completed due to the inability of conversion rates and selectivity to meet the industrialization requirements.A better understanding of the reaction mechanism and the development of highefficiency and high-selectivity electrocatalysts are required to pave the path toward larger industrialization ***,we summarize the recent research progress in the electrocatalytic oxidation and hydrogenation of platform compounds such as furanic compounds and *** the literature,these three research areas are integrated to realize the scale-up application of the processes as mentioned *** investigations of the mechanism are based on in situ techniques,theoretical calculations,and advanced electrocatalyst ***,the challenges and prospects in this topic are *** expect that this review will provide the fundamental understanding and design guidelines to achieve efficient and high-selectivity catalysts and further facilitate the scale-up application of the electrocatalytic conversion of biomass derivatives.

关键词： electrocatalyst electrochemical hydrogenation electrochemical oxidation furanic compound glycerol

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Low-temperature plasma technology for electrocatalysis

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Chinese chemical Letters 2019年第4期30卷 826-838页

作者： Dongdong Wang Yuqin Zou Li Tao Yiqiong Zhang Zhijuan Liu Shiqian Du Shuangquan Zang Shuangyin Wang State key laboratory of chem/bio-sensing and chemometrics Provincial Hunan Key Laboratory for Graphene Materials and Devices College of Chemistry and Chemical Engineering Hunan University College of chemistry and Molecular Engineering Zhengzhou University

Electrochemical reactions were widely used in energy storage and conversion devices. The development of low-cost, highly efficient and stable electrocatalyst is essential to a large-scale application of energy storage and conversion devices. Recently, emerging plasma technology has been employed as one of the practical ways to synthesize and modify electrocatalysts due to its unique property. In this review, we summarized the latest applications of plasma in energy storage and conversion, including using it as the preparation and modification technology of the various electrocatalysts and the usage of it as the synthesis technology directly. Firstly, we presented the definition and types of plasma reactors and their respective characteristics. Then, these applications of plasma technology in many essential electrode reactions including carbon dioxide reduction reaction(CO_2RR), nitrogen fixation, oxygen reduction reaction(ORR), oxygen evolution reaction(OER) and hydrogen evolution reaction(HER) were ***, the challenges and outlook of plasma technology in energy storage and conversion were summarized, and the solutions and prospected its development in the future were present. Through reviewing the related aspects, readers can have a deeper understanding of the application prospects of plasma in electrocatalysis.

关键词： Plasma Electrocatalysts Electrode reactions Energy storage Energy conversion

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