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Plasmon-induced local electric field improved hydrogen evolution reaction on Ag/Mo_(2)C nanosheets

Nano Research 2025年第1期18卷 270-277页

作者： huangjingwei li Xin Zi Jun Wu Xinli Wang li Zhu Qiyou Wang Jianfu Han Junwei Fu Hongmei li Kai Huang Yu Chen Min liu School of Physics State Key Laboratory of Powder MetallurgyHunan Joint International Research Center for Carbon Dioxide Resource UtilizationCentral South UniversityChangsha 410083China School of Metallurgy and Environment Central South UniversityChangsha 410083China Institute of High Energy Physics Chinese Academy of Sciences(CAS)Beijing 100049China Nano-Institute Munich Faculty of PhysicsLudwig-Maxilimians-Universität MünchenMünchen 80539Germany Hunan Institute of Advanced Sensing and Information Technology Xiangtan UniversityXiangtan 411105China

Electrocatalytic water splitting offers a promising way for hydrogen production with near-zero ***,such as molybdenum carbides(Mo_(2)C),are promising materials for hydrogen evolution reaction(HER)but still suffer from poor intrinsic water activation ***,we developed a plasmon-induced local electric field(PILEF)strategy to solve this ***(Ag)nanoparticles decorated Mo_(2)C nanosheets(Ag/Mo_(2)C)were successfully prepared by electrostatic *** visible light excited the PILEF on Ag/Mo_(2)C remarkably reducing the activation energy by 92.7 kJ·mol^(-1)from 147.3 kJ·mol^(-1)of Mo_(2)C to 54.6 kJ·mol^(-1).As a result,the plasmonic Ag/Mo_(2)C significantly enhances~2.3-fold of the current density from 2.8 mA·cm^(-2)of Mo_(2)C to 6.5 mA·cm^(-2)at-3 V *** and reduces the overpotential by 104 mV from 403 mV of dark state to 299 mV of light state at the current density of 10 mA·cm^(-2),achieving better performance than reported *** research demonstrates that PILEF enhances HER activities,offering a potential strategy for boosting the intrinsic activities of catalysts.

关键词： sliver particles plasmon effect field effect hydrogen evolution reaction(HER) electrocatalysis

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Sequential reactant water management by complementary multisite catalysts for surpassing platinum hydrogen evolution activity

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Nano Research 2024年第3期17卷 1232-1241页

作者： Yu lin Defang Ding Shicheng Zhu Qunlei Wen huangjingwei li Zhen li Youwen liu Yi Shen China Engineering Research Center of Nano-Geomaterials of Ministry of Education Faculty of Materials Science and ChemistryChina University of GeosciencesWuhan 430078China State Key Laboratory of Materials Processing and Die&Mould Technology and School of Materials Science and EngineeringHuazhong University of Science and TechnologyWuhan 430074China

Alkaline hydrogen evolution reaction(HER)offers a near-zero-emission approach to advance hydrogen ***,the activity limited by the multiple reaction steps involving H_(2)O molecules transfer,absorption,and activation still unqualified the thresholds of economic ***,we proposed a multisite complementary strategy that incorporates hydrophilic Mo and electrophilic V into Ni-based catalysts to divide the distinct steps on atomically dispersive sites and thus realize sequential regulation of the HER *** Isotopic labeled in situ Raman spectroscopy describes 4-coordinated hydrogen bonded H_(2)O to be free H_(2)O passing the inner Helmholtz plane in the vicinity of the catalysts under the action of hydrophilic Mo ***,potential-dependent electrochemical impedance spectroscopy(EIS)reveals that electrophilic V sites with abundant 3d empty orbitals could activate the lone-pair electrons in the free H_(2)O molecules to produce more protic hydrogen,and dimerize into H_(2) at the Ni *** the sequential management of reactive H_(2)O molecules,NiMoV oxides multisite catalysts surpass Pt/C hydrogen evolution activity(49 mV@10 mA∙cm^(-2) over 140 h).Profoundly,this study provides a tangible model to deepen the comprehension of the catalyst–electrolyte interface and create efficient catalysts for diverse reactions.

关键词： hydrogen evolution activity complementary multisite catalysts sequential reactive water management interfacial water molecules

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Regulating local charges of atomically dispersed Moδ+ sites by nitrogen coordination on cobalt nanosheets to trigger water dissociation for boosted hydrogen evolution in alkaline media

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Journal of Energy Chemistry 2022年第9期31卷 125-132,I0004页

作者： Maoqi Cao Kang liu Yao Song Chao Ma Yiyang lin huangjingwei li Kejun Chen Junwei Fu Hongmei li Jun Luo Yida Zhang Xusheng Zheng Junhua Hu Min liu School of Chemistry and Chemical Engineering Qiannan Normal University for NationalitiesDuyun 558000GuizhouChina State Key Laboratory of Powder Metallurgy School of Physics and ElectronicsShenzhen Research InstituteSchool of Physical and ElectronicsCentral South UniversityChangsha 410083HunanChina School of Materials Science and Engineering Central South University of Forestry and TechnologyChangsha 410004HunanChina School of Materials Science and Engineering Hunan UniversityChangsha 410082HunanChina National Synchrotron Radiation Laboratory University of Science and Technology of ChinaHefei 230029AnhuiChina School of Materials Science and Engineering Zhengzhou UniversityZhengzhou 450001HenanChina

Now,Pt-based materials are still the best catalysts for hydrogen evolution reaction(HER).Nevertheless,the scarcity of Pt makes it impossible for the large-scale applications in *** cobalt is taken as an excellent HER catalyst due to its suitable H*binding,its alkali HER catalytic property need to be improved because of the sluggish water dissociation *** this work,nitrogen with small atomic radius and metallophilicity is employed to adjust local charges of atomically dispersed Mo^(δ+)sites on Co nanosheets to trigger water *** calculations suggest that the energy barrier of water dissociation can be effectively reduced by introducing nitrogen coordinated Mo^(δ+)*** realize this speculation,atomically dispersed Mo^(δ+)sites with nitrogen coordination of Mo(N)/Co were prepared via reconstruction of CoMoO_(4).High angle annular dark-field scanning transmission electron microscopy(HAADF-STEM)and X-ray absorption spectroscopy(XAS)demonstrate the coordination of N atoms with atomically dispersed Mo atoms,leading to the local charges of atomically dispersed Mo^(δ+)sites in Mo(N)/*** measurement from ambient pressure X-ray photoelectron spectroscopy(AP-XPS)reveals that the Mo^(δ+)sites promote the adsorption and activation of water ***,the Mo(N)/Co exhibits an excellent activity,which need only an overpotential of 39 mV to reach the current density of 10 mA cm^(-2).The proposed strategy provides an advance pathway to design and boost alkaline HER activity at the atomic-level.

关键词： Charge localized Mo Nitrogen coordination Co nanosheet Water dissociation Alkaline HER

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Graphitic carbon nitride based single-atom photocatalysts

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Frontiers of physics 2020年第3期15卷 13-26,M0001页

作者： Junwei Fu Shuandi Wang Zihua Wang Kang liu huangjingwei li Hui liu Junhua Hu Xiaowen Xu Hongmei li Min liu School of Physics and Electronics State Key Laboratory of Powder MetallurgyHunan Provincial Key Laboratory of Chemical Power SourcesCentral South UniversityChangsha410083China School of Metallurgy and Environment Central South UniversityChangsha410083China School of Materials Science and Engineering Zhengzhou UniversityZhengzhou450002China

Single-atom photocatalysts,due to their high catalysis activity,selectivity and stability,become a hotspot in the field of *** carbon nitride(g-C3N4)is known as both a good support for single atoms and a star *** g-C3N4-based single-atom photocatalysts exhibits great potential in improving the photocatalytic *** this review,we summarize the recent progress in g-C3N4-based single-atom photocatalysts,mainly including preparation strategies,characterizations,and their photocatalytic *** significant roles of single atoms and catalysis mechanism in g-C3N4-based single-atom photocatalysts are *** last,the challenges and perspectives for exploring high-efficient g-C3N4-based single-atom photocatalysts are presented.

关键词： graphitic carbon nitride single atoms atomically dispersed sites site-isolated catalysts photocatalysis

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Electric-field promoted C–C coupling over Cu nanoneedles for CO_(2) electroreduction to C_(2) products

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Chinese Journal of Catalysis 2022年第2期43卷 519-525页

作者： huangjingwei li Huimin Zhou Yajiao Zhou Junhua Hu Masahiro Miyauchi Junwei Fu Min liu Hunan Provincial Key Laboratory of Chemical Power Sources State Key Laboratory of Powder MetallurgySchool of Physics and ElectronicsCentral South UniversityChangsha 410083HunanChina School of Materials Science and Engineering Zhengzhou UniversityZhengzhou 450002HenanChina Department of Materials Science and Engineering School of Materials and Chemical TechnologyTokyo Institute of TechnologyTokyo 152-8552Japan

Cu-based catalysts are the most promising candidates for electrochemical CO_(2)reduction(CO_(2)RR)to multi-carbon(C_(2))*** the C-C coupling process,the rate-determining step for C_(2)product generation,is an important strategy to improve the production and selectivity of the C_(2)*** this study,we determined that the local electric field can promote the C-C coupling reaction and enhance CO_(2)electroreduction to C_(2)***,finite-element simulations indicated that the high curvature of the Cu nanoneedles results in a large local electric field on their *** functional theory(DFT)calculations proved that a large electric field can promote C-C *** by this prediction,we prepared a series of Cu catalysts with different *** Cu nanoneedles(NNs)exhibited the largest number of curvatures,followed by the Cu nanorods(NRs),and Cu nanoparticles(NPs).The Cu NNs contained the highest concentration of adsorbed K+,which resulted in the highest local electric field on the *** adsorption sensor tests indicated that the Cu NNs exhibited the strongest CO adsorption ability,and in-situ Fourier-transform infrared spectroscopy(FTIR)showed the strongest*COCO and*CO signals for the Cu *** experimental results demonstrate that high-curvature nanoneedles can induce a large local electric field,thus promoting C-C *** a result,the Cu NNs show a maximum FEC_(2)of 44%for CO_(2)RR at a low potential(-0.6 V ***),which is approximately 2.2 times that of the Cu *** work provides an effective strategy for enhancing the production of multi-carbon products during CO_(2)RR.

关键词： Electric-field effect C–C coupling Cu nanoneedle C_(2)products CO_(2)electroreduction

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Tuning the electron structure enables the NiZn alloy for CO_(2) electroreduction to formate

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Journal of Energy Chemistry 2021年第12期30卷 625-632,I0015页

作者： Xiaodong Zhang Yajiao Zhou Hang Zhang Huang Jing Wei li Kang liu Hongmei li Hao Pan Junhua Hu Junwei Fu Shanyong Chen Min liu School of Physics and Electronics Hunan Provincial Key Laboratory of Chemical Power SourcesState Key Laboratory of Powder MetallurgyCentral South UniversityChangsha 410083HunanChina Department of Periodontics&Oral Mucosal Section Xiangya Stomatological HospitalCentral South UniversityChangsha 410008HunanChina School of Materials Science and Engineering Zhengzhou UniversityZhengzhou 450002HenanChina School of Environment Guangdong Key Laboratory of Environmental Pollution and HealthJinan UniversityGuangzhou 511443GuangdongChina

Formate is an important liquid chemical,which can be produced by electrocatalytic carbon dioxide reduction reaction(CO_(2) RR).Most of the metal catalysts for CO_(2) RR to formate are toxic or noble metals,such as Cd,Hg,Pb and Pd,leading to the environmental pollution or increased production ***,we develop an environmentally friendly and low-cost NiZn alloy catalyst for CO_(2) RR to *** X-ray diffraction(XRD),X-ray photoelectron spectroscopy(XPS) and transmission electron microscopy(TEM) confirm the alloy structure of the prepared NiZn catalyst. As for a catalyst for CO_(2) RR,the NiZn alloy exhibits the FE_(HCOO)^(-)(Faraday efficiency of HCOO^(-)) of 36±0.7% at-0.9 V *** in 0.1 M KHCO_(3), and remarkable stability for 40,000 s at-0.8,-0.9,-1.0 and-1.1 V ***,*** calculation results indicate that the NiZn alloy exhibits the middle valence electron structure between the Zn and Ni metal,resulting in the favorable pathway for HCOOH formation but unfavorable for the hydrogen evolution reaction and CO *** Ultraviolet Photoelectron Spectroscopy results verify the modulated valence electron structure for NiZn alloy as compared to Ni and Zn,consistent with the theoretical calculation *** work provides new insights into design of alloy catalysts for CO_(2) RR to formate.

关键词： Electrocatalysis CO_(2)reduction reaction Formate NiZn alloy Valence electron structure

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外场驱动分子极化调控反应物界面及其电催化析氢性能

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Science China Materials 2023年第9期66卷 3501-3508页

作者：赵阳黄家钊陈建强干晓娟温群磊李黄经纬段君元陈搏文翟天佑刘友文 School of Materials Science and Engineering Huazhong University of Science and TechnologyWuhan 430074China

反应物界面对电催化反应至关重要.然而,由于调控和表征手段的不足,对反应物界面的深入研究仍难以实现.本文中,我们借助单片电催化微纳器件,通过调节背栅电压引入分子极化,实现了对电化学双电层中水合氢离子(H_(3)O^(+))浓度的调控,进而... 详细信息

反应物界面对电催化反应至关重要.然而,由于调控和表征手段的不足,对反应物界面的深入研究仍难以实现.本文中,我们借助单片电催化微纳器件,通过调节背栅电压引入分子极化,实现了对电化学双电层中水合氢离子(H_(3)O^(+))浓度的调控,进而提高了催化剂的电催化析氢性能.以C_(60)/MoS_(2)异质结为例,电学性能测试表明背栅电场促进了电子从C_(60)向MoS_(2)的转移,并导致了C_(60)分子的极化.原位光致发光光谱表征显示,在背栅电场的作用下,极化的C_(60)分子会吸引H_(3)O^(+),使其聚集在MoS_(2)附近.而电催化测试表明,在1.5 V背栅电压下,由于发生了H_(3)O^(+)的富集,C_(60)/MoS_(2)异质结在-0.45 VRHE电位下的析氢电流密度增加了5倍我们提出的调控和监测反应物界面的方法能够促进对多种电催化反应的研究.

关键词：光致发光光谱电催化水合氢离子电化学分子极化异质结双电层微纳器件

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