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Regulation of the pore structure of carbon nanosheets based Electrocatalyst for efficient polysulfides phase conversions

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Journal of Materials Science & Technology 2024年第4期171卷 37-46页

作者： Xiaoyang Liu Jingbo Zhang Kangli Liu Shijie Zhang Rouhan Hou Xiaoyi Hu Peng Zhang Guosheng Shao State Center for International Cooperation on Designer Low-Carbon&Environmental Materials(CDLCEM) School of Materials Science and EngineeringZhengzhou UniversityZhengzhou 450001China Zhengzhou Materials Genome Institute(ZMGI) Xingyang 450100China

The practical applications of lithium-sulfur(Li-S)batteries are hampered by the sluggish redox kinetics and polysulfides shuttle in the cyclic process,which leads to a series of problems including the loss of active materials and poor cycling efficiency.In this paper,the pore structures of carbon nanosheets based Electrocatalysts were precisely controlled by regulating the content of water-soluble KCl template.The relationship between pore structures and Li-S electrochemical behavior was studied,which demonstrates a key influence of pore structure in polysulfides phase conversions.In the liquid-sloid redox reaction of polysulfides,the micropores and small mesopores(d20 nm)and macropores played a decisive role.As a typical exhibition,the nickel-embedded carbon nanosheets(Ni-CNS)with a high content of large mesopores and macropores can aid Li-S batteries in exhibiting stable cycling performance(760.1 mAh g^(-1)at 1 C after 300 cycles)and superior rate capac-ity(847.8 mAh g^(-1)at 2 C).Furthermore,even with high sulfur loading(8 mg cm^(−2))and low electrolyte(E/S is around 6μL mg^(-1)),the high area capacity of 7.7 mAh cm^(−2)at 0.05 C could be achieved.This work can provide a guideline for the design of the pore structure of carbon-based Electrocatalysts toward high-efficiency sulfur species redox reactions,and afford a general,controllable,and simple approach to constructing high performance Li-S batteries.

关键词： Hierarchical porous carbon network Electrocatalyst Molten salt templating method Modified separators Li-S batteries

Coordinately unsaturated nickel single atom Electrocatalyst for efficient CO_(2)conversion

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Nano Research 2023年第8期16卷 10873-10880页

作者： Wei Zhang Dong Liu Tong Liu Chenglong Ding Tao Chen Yanming Li Xiaokang Liu Lan Wang Changli Li Jingfu He Tao Ding Tao Yao School of Materials Sun Yat-Sen UniversityGuangzhou 510275China National Synchrotron Radiation Laboratory University of Science and Technology of ChinaHefei 230029China School of National Defense Science and Technology Southwest University of Science and TechnologyMianyang621010China

Single-atom catalysts(SACs)have shown unexpected catalytic activity due to their unique electronic structure and coordination environment.Nonetheless,the synthesis of an atomically precise low-coordination single-atom catalyst remains a grand challenge.Herein,we report a coordinately unsaturated Ni-N_(3)single-atom Electrocatalyst using a metal-organic framework(MOF)derived N-C support with abundant exposed N for excellent electrochemical CO_(2)reduction.The obtained Ni-N_(3)/NC active site exhibited highly efficient CO_(2)-to-CO conversion with a Faradaic efficiency of 94.6%at the current density of 100 mA/cm^(2).In situ X-ray absorption spectroscopy(XAS)measurement suggested that the Ni atomic center with unsaturated coordination had the lower initial chemical state and higher charge transfer ability.In situ Fourier transform infrared(FT-IR)and theoretical calculation results revealed that the unsaturated catalytically active center could facilitate activation of CO_(2)and thus heighten CO_(2)electroreduction activity.These findings provided insights into the rational design of definitive coordination structure of SACs for boosting activity and selectivity.

关键词： Ni single atom Electrocatalyst in situ X-ray absorption spectroscopy in situ Fourier transform infrared

Inverted-design for highly-active hydrogen evolution Electrocatalyst of MoS_(2)@Ni_(3)S_(2)core-shell via unlocking the potential of Mo

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颗粒学报:英文版 2023年第6期77卷 56-61页

作者： Chao Song Yuhua Liu Chengxiang Huang Miao Liu Nailin Yue Zunhao Zhang Zizhun Wang Xu Zou Wei Zhang Weitao Zheng Key Laboratory of Automobile Materials MOE School of Materials Science&EngineeringJilin Provincial International Cooperation Key Laboratory of High-Efficiency Clean Energy MaterialsElectron Microscopy CenterInternational Center of Future ScienceJilin UniversityChangchun130012China

Through inverted-design rather than modifying the generally-assumed S active sites in popular MoS_(2),we unlock the potential of Mo sites and successfully prepared novel MoS_(2)@Ni_(3)S_(2)/NF core-shell nanospheres as a catalyst for the high-performance hydrogen evolution reaction(HER).TheΔGH at the Mo site is optimized via Ni_(3)S_(2)to achieve excellent HER activity.At low current densities,it has similar activity to the Pt/C.However,its performance is better than Pt/C at high density.Moreover,our catalyst shows a considerable stability at a variety of current densities for 50 h,promising to substitute noble metal catalysts in application of commercial alkaline Electrocatalysts.

关键词： Inverted design Hydrogen evolution reaction Electrocatalyst Electronicinteraction MoS_(2)@Ni_(3)S_(2)/NF

Co-doped Ni_(3)S_(2) nanosheet array: A high-efficiency Electrocatalyst for alkaline seawater oxidation

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Nano Research 2024年第3期17卷 1050-1055页

作者： Meng Yue Xun He Shengjun Sun Yuntong Sun Mohamed S.Hamdy Mhamed Benaissa Alsamani A.M.Salih Jun Liu Xuping Sun College of Chemistry Chemical Engineering and Materials ScienceShandong Normal UniversityJinan 250014China Institute of Fundamental and Frontier Sciences University of Electronic Science and Technology of ChinaChengdu 610054China Department of Chemistry College of ScienceKing Khalid UniversityP.O.Box 9004Abha 61413Saudi Arabia Department of Chemical Engineering College of EngineeringUniversity of Ha’ilP.O.Box 2440Ha’il 81441Saudi Arabia Department of Otolaryngology-Head&Neck Surgery West China HospitalSichuan UniversityChengdu 610041China

Developing efficient and durable oxygen evolution reaction(OER)catalysts holds great promise for green hydrogen production via seawater electrolysis,but remains a challenge.Herein,we report a Co-doped Ni_(3)S_(2) nanosheet array on Ni foam(Co-Ni_(3)S_(2)/NF)as a high-efficiency OER Electrocatalyst for seawater.In alkaline conditions,Co-Ni_(3)S_(2)/NF requires an overpotential of only 368 mV to drive 100 mA·cm^(–2),superior to Ni_(3)S_(2)/NF(385 mV).Besides,it exhibits at least 50-h continuous electrolysis.

关键词： Co doping Ni_(3)S_(2)nanosheet array oxygen evolution reaction seawater electrolysis Electrocatalyst

具有优越电催化析氢性能的超小碳负载FeRu合金

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Science China Materials 2023年第7期66卷 2672-2679页

作者：刘国华张照艳刘文宁杨文昕安丽曲丹刘弈畅汪夏燕孙再成 Center of Excellence for Environmental Safety and Biological Effects Beijing Key Laboratory for Green Catalysis and SeparationDepartment of ChemistryFaculty of Environment and LifeBeijing University of TechnologyBeijing 100124China

电化学水分解是将可再生能源产生的间歇性电能转化为高纯度氢气的一种极具前景的绿色能源技术.目前,高效制氢催化剂主要由贵金属及其化合物组成,而贵金属的高成本及稀缺性,限制了其在大规模工业化制氢中的应用.因此,探索低成本,高电化... 详细信息

电化学水分解是将可再生能源产生的间歇性电能转化为高纯度氢气的一种极具前景的绿色能源技术.目前,高效制氢催化剂主要由贵金属及其化合物组成,而贵金属的高成本及稀缺性,限制了其在大规模工业化制氢中的应用.因此,探索低成本,高电化学活性、高稳定性的电解水制氢催化剂至关重要.合金化材料以短程或长程有序结构存在,具有增强的电化学性能.因此,本文采用两步法制备超小碳负载FeRu合金纳米电催化剂并将其应用于电催化析氢反应.Fe_(0.05)Ru_(0.05)/XC-72双功能电催化剂粒径为2.1 nm,在碱性淡水和海水电解质中表现出优异的活性和耐久性.10 mA cm^(-2)时,在1 mol L^(-1)KOH、1 mol L^(-1)KOH+0.5 mol L^(-1)NaCl和1 mol L^(-1)KOH+海水中分别表现出13、15和18 mV的过电位.在1 mol L^(-1)KOH介质和-0.07 V(相比于可逆氢电极)条件下,Fe_(0.05)Ru_(0.05)/XC-72的析氢质量活性高达11.32Amg^(-1)_(noble metal).在1 mol L^(-1)KOH中,Fe_(0.05)Ru_(0.05)/XC-72电催化剂具有24 h以上的长期析氢反应(HER)稳定性.理论计算表明,引入Fe形成的FeRu合金可以诱导电子效应,使其对*H的吸附能力增强,进一步提高了HER性能.本工作对制备高电活性、高稳定性的钌基电催化剂具有重要的启发意义.

关键词： FeRu alloy Electrocatalyst hydrogen evolution reaction electronic effect

Polyoxometalates-derived ternary metal oxides Electrocatalyst for N_(2) reduction under ambient conditions

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Tungsten 2024年第2期6卷 428-437页

作者： Meng-Le Yang Zhong-Xin Jin Xi-Xian Cao Xin-Ming Wang Hui-Yuan Ma Hai-Jun Pang Gui-Xin Yang The School of Material Science and Chemical Engineering Harbin University of Science and TechnologyHarbin 150040China

Accelerating the breaking of the nitrogen nonpolar bond(N≡N)is an important factor to improve the effi ciency of the electro-catalytic nitrogen reduction reaction(e-NRR).In this work,polyoxometalates-derived FeMo-based ternary oxide materials MoO_(2)-Mo_(4)O_(11)-FeMoO_(4)@X(abbreviated as MoFeO@X,X represents the synthesis temperature of 650,750 and 850℃)were designed and synthesized for e-NRR under ambient conditions.The scanning electron microscopy images of MoFeO@750 show an ellipsoidal-like structure(0.86×0.6μm).The relatively large specifi c surface area,formation of multiple interfaces,together with the synergistic eff ect of iron and molybdenum bimetals,would make MoFeO@X catalyst more easily absorb and activate N_(2)in the e-NRR.Expectedly,the synthesized MoFeO@750 shows an optimal NH_(3)production rate of 16.57μg·h^(−1)·mg cat.^(−1)and Faradaic effi ciency of 12.33%at−0.3 V versus reversible hydrogen electrode(νs.RHE),with outstanding electrochemical and structural stability.

关键词： Polyoxometalates Electrocatalytic nitrogen reduction reaction Ternary oxide Electrocatalyst

In situ growth of phosphorized ZIF-67-derived amorphous CoP/Cu_(2)O@CF Electrocatalyst for efficient hydrogen evolution reaction

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Frontiers of Chemical Science and Engineering 2023年第10期17卷 1430-1439页

作者： Ruiwen Qi Xiao Liu Hongkai Bu Xueqing Niu Xiaoyang Ji Junwei Ma Hongtao Gao Key Laboratory of Optic-Electric Sensing and Analytical Chemistry for Life Sciences MOECollege of Chemistry and Molecular EngineeringQingdao University of Science and TechnologyQingdao 266042China

Transition metal phosphides have been extensively studied for catalytic applications in water splitting.Herein,we report an in situ phosphorization of zeolitic imidazole frameworks(ZIF-67)to generate amorphous cobalt phosphide/ZIF-67 heterojunction on a self-supporting copper foam(CF)substrate with excellent performance for hydrogen evolution reaction(HER).The needleleaf like copper hydroxide was anchored on CF surface,which acted as implantation to grow ZIF-67.The intermediate product was phosphorized to obtain final Electrocatalyst(CoP/Cu_(2)O@CF)with uniform particle size,exhibiting a rhombic dodecahedron structure with wrinkles on the surface.The electrochemical measurement proved that CoP/Cu_(2)O@CF catalyst exhibited excellent HER activity and long-term stability in 1.0 mol·L^(–1)KOH solution.The overpotential was only 62 mV with the Tafel slope of 83 mV·dec^(–1)at a current density of 10 mA·cm^(–2),with a large electrochemical active surface area.It also showed competitive performance at large current which indicated the potential application to industrial water electrolysis to produce hydrogen.First-principle calculations illustrated that benefit from the construction of CoP/ZIF-67 heterojunction,the d-band center of CoP downshifted after bonding with ZIF-67 and the Gibbs free energy(ΔGH*)changed from–0.18 to–0.11 eV,confirming both decrease in overpotential and excellent HER activity.This work illustrates the efficient HER activity of CoP/Cu_(2)O@CF catalyst,which will act as a potential candidate for precious metal Electrocatalysts.

关键词： CoP/Cu_(2)O@CF Electrocatalyst phosphorization HER DFT

High-entropy alloy nanoparticles as a promising Electrocatalyst to enhance activity and durability for oxygen reduction

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Nano Research 2022年第9期15卷 7868-7876页

作者： Yanan Yu Fanjie Xia Chengjie Wang Jinsong Wu Xianbiao Fu Dongsheng Ma Bencai Lin Jiaao Wang Qin Yue Yijin Kang Institute of Fundamental and Frontier Sciences University of Electronic Science and Technology of ChinaChengdu 610054China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Nanostructure Research CenterWuhan University of TechnologyWuhan 430070China Jiangsu Province Cultivation base for State Key Laboratory of Photovoltaic Science and Technology Changzhou UniversityChangzhou 213164China Department of Chemistry and the Oden Institute for Computational Engineering and Sciences The University of Texas at AustinTX 78712USA

Developing efficient platinum-based Electrocatalysts with super durability for the oxygen reduction reaction(ORR)is highly desirable to promote the large-scale commercialization of fuel cells.Although progress has been made in this aspect,the electrochemical kinetics and stability of platinum-based catalysts are still far from the requirements of the practical applications.Herein,PtPdFeCoNi high-entropy alloy(HEA)nanoparticles were demonstrated via a high-temperature injection method.PtPdFeCoNi HEA nanocatalyst exhibits outstanding catalytic activity and stability towards ORR due to the high entropy,lattice distortion,and sluggish diffusion effects of HEA,and the HEA nanoparticles delivered a mass activity of 1.23 A/mgPt and a specific activity of 1.80 mA/cmPt 2,which enhanced by 6.2 and 4.9 times,respectively,compared with the values of the commercial Pt/C catalyst.More importantly,the high durability of PtPdFeCoNi HEA/C was evidenced by only 6 mV negativeshifted half-wave potential after 50,000 cycles of accelerated durability test(ADT).

关键词： high-entropy alloy oxygen reduction reaction Electrocatalyst high durability

Sulfurization accelerator coupled Fe_(1-x)S Electrocatalyst boosting SPAN cathode performance

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Nano Research 2023年第7期16卷 9231-9239页

作者： Jinlei Qin Yun Lu Rui Wang Zhizhan Li Tao Shen Deli Wang Key Laboratory of Materials Chemistry for Energy Conversion and Storage of Ministry of Education Hubei Key Laboratory of Material Chemistry and Service FailureSchool of Chemistry and Chemical EngineeringHuazhong University of Science and TechnologyWuhan 430074China

Sulfurized polyacrylonitrile(SPAN)cathode exhibits improved cycling stability in carbonate electrolytes due to the existent of-S_(x)^(2-)-(2≤n≤4)units.However,it is still challenging for SPAN to achieve higher sulfur content,superior conductivity,and faster polysulfide conversion kinetics in ether electrolytes.Herein,polyacrylonitrile(PAN),2-morpholinothiobenzothiazole(MBS),and FeCl_(3)coated reduced graphene oxide(rGO)were used to fabricate advanced sulfur cathode through electrospinning technology to address these problems.During PAN sulfuration reactions,the MBS with abundant unsaturated bonds served as the vulcanization accelerator to facilitate the formation of longer chain sulfur species(-S_(3)-/-S_(4)-)and increase the sulfur content in the SPAN electrode system.Meanwhile,Fe_(1-x)S is in situ converted from FeCl_(3),which acts as the Electrocatalyst to promote Li_(2)S nucleation and decomposition reactions.As a result,the Fe_(1-x)S/SPAN/rGO electrode with high sulfur loading of 2.0 mg·cm^(-2)delivers a reversible capacity of 1122 mAh·g^(-1)at 0.1 A·g^(-1).Notably,at a large current density of 5.0 A·g^(-1),the Fe_(1-x)S/SPAN/rGO electrode still displays a high specific capacity of 924 mAh·g^(-1)with an ultra-stable cycling life over 2000 cycles.The present work provides new insights into designing of high-performance electrode materials for long-lasting Li-S batteries.

关键词： Li-S batteries Electrocatalyst electrospun sulfurized polyacrylonitrile(SPAN) vulcanization accelerators