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Nano Research 2023年第5期16卷 7941-7949页

作者： Xinmei Liu Xue Li Wenlong Yang Gang Liu Yu Wang Yuhang Zuo Harbin University of Science and Technology Harbin 150001China Jiangsu Zhongsheng Gaoke Environment Co. Ltd.Wuxi 214244China

High cost and restricted activity of electrocatalysis are the major challenges for hydrogen generation and biosensors.In this work,we provided a one-pot synthesis of Cu_(x)Pd_(y)alloy nanoparticles(NPs)with controllable atomic ratio and“clean surface”.Benefiting from the preferable d-band structure,the Cu_(62)Pd_(38)NPs exhibited a lower overpotentials in the hydrogen evolution reaction(HER)over the full pH range.In the acidic media,Cu_(62)Pd_(38)NPs achieved a low overpotential of 28.12 mV for HER,which was 25.73%of Pd NPs.In the neutral solution,the overpotential by Cu_(62)Pd_(38)NPs is only 41.71%for that by uncleaned CuPd NPs.In alkaline media,the overpotential by Cu_(62)Pd_(38)NPs was declined from 38.01 to 20.20 mV after 720 min yielding hydrogen,which was only 53.14%for the initial overpotential.As applied in biosensor,the synergistic effect of Cu and Pd accelerated the kinetics of electrocatalytic process,resulting in an enhanced performance.The glucose sensor constructed by Cu_(67)Pd_(33)exhibited a wider detection range up to 100.0 mM.And the sensitivity is 379.4μA/(mM·cm^(2)),which is ca.4.63 and 14.09 folds for that by pure Cu NPs and Pd NPs,respectively.An optimal atomic percent would be conducive to optimize electrocatalytic activity of Cu_(x)Pd_(y)alloy.The volcano plots for Cu_(x)Pd_(y)would open up a new avenue for designing electrocatalysis with rationalized cost and optimized performance.

关键词： alloy biosensor hydrogen evolution reaction overpotential detection range

Improving the water electrolysis performance by manipulating the generated nano/micro-bubbles using surfactants

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Nano Research 2023年第1期16卷 420-426页

作者： Houpeng Wang Zhaoxiang Xu Wei Lin Xue Yang Xianrui Gu Wei Zhu Zhongbin Zhuang SINOPEC Research Institute of Petroleum Processing Beijing 100083China State Key Lab of Organic-Inorganic Composites and Beijing Advanced Innovation Center for Soft Matter Science and Engineering Beijing University of Chemical TechnologyBeijing 100029China Beijing Key Laboratory of Energy Environmental Catalysis Beijing University of Chemical TechnologyBeijing 100029China

The impeded mass transfer rate by on-site-generated gas bubbles at both cathode and anode dramatically reduces the energy conversion efficiency of the proton exchange membrane water electrolyzer(PEMWE).Herein,we report a surfactant-assistant method to accelerate the nano/micro-bubble detachment and the mass transfer rate by reducing the surface tension,resulting in an increase in overall efficiency.Four kinds of surfactants are studied in this work.Only potassium perfluorobutyl sulfonate(PPFBS),which has the structural similarity to Nafion,shows a significant promotion of activity and stability for both hygrogen evolution reaction(HER)and oxygen evolution reaction(OER)in the acidic medium at the high current density region.The HER overpotential at 0.1 A·cm−2 decreased 22%,and the current density at−0.4 V increased 31%by adding PPFBS.The promotion of overall efficiency by PPFBS on a homemade PEMWE was also proven.The reduced surface tension and electrostatic repulsion were the probable origins of the accelerated bubble detachment.

关键词： proton exchange membrane water electrolysis bubble overpotential surfactant electrostatic repulsion

Ag nanoparticles anchored on MIL-100/nickel foam nanosheets as an electrocatalyst for efficient oxygen evolution reaction performance

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Chinese Journal of Chemical Engineering 2022年第1期35卷 480-487页

作者： Tao Zhao Dazhong Zhong Genyan Hao Guang Liu Jinping Li Qiang Zhao Shanxi Key Laboratory of Gas Energy Efficient and Clean Utilization College of Chemistry and Chemical EngineeringTaiyuan University of TechnologyTaiyuan 030024China

Metal-organic frameworks(MOFs)exhibit excellent application potential in the field of electrocatalysis.In this study,we first prepare MIL-100 nanosheets on nickel foam(MIL-100/NF)and then successfully anchor Ag nanoparticles(NPs)on the nanosheets(Ag@MIL-100/NF)for oxygen evolution reaction(OER)catalysis.This strategy dramatically improves the conductivity of MIL-100 and the Ag NPs are uniformly dispersed on the nanosheets.The Ag@MIL-100/NF catalyst has excellent electrocatalytic performance and long-term corrosion resistance,with a low overpotential of 207 mV and a long-term stability of at least 100 h at a current density of 50 mA·cm^(-2).The experimental results demonstrate that this high OER catalytic performance is due to the improved charge transfer after loading Ag NPs,the combination of nanosheets and highly dispersed Ag NPs that expose more active sites and the adjusted chemical valence states of Fe and Ni in MIL-100.This work provides a surface decoration approach for the preparation of excellent catalysts directly used in the OER.

关键词： Ag@MIL-100/NF Metal-organic frameworks Catalysis Kinetics overpotential Electrochemistry

Revealing the illumination effect on the discharge products in high-performance Li-O_(2) batteries with heterostructured photocatalysts

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Carbon Energy 2022年第6期4卷 1169-1181页

作者： Hao Gong Tao Wang Kun Chang Peng Li Lequan Liu Xingyu Yu Bin Gao Hairong Xue Renzhi Ma Jianping He Jinhua Ye Department of Chemistry and Materials Science College of ScienceNanjing Forestry UniversityNanjingChina Jiangsu Key Laboratory of Materials and Technology for Energy Conversion College of Materials Science and TechnologyNanjing University of Aeronautics and AstronauticsNanjingChina TJU-NIMS International Collaboration Laboratory School of Material Science and EngineeringTianjin UniversityTianjinChina International Center for Materials Nanoarchitectonics(WPI-MANA) National Institute for Materials Science(NIMS)IbarakiJapan

Aprotic lithium–oxygen batteries(LOBs)have been recognized as novel energy storage devices for their outstanding specific energy density,while the large discharge/charge overpotential is a tough barrier to be overcome.Here,hetero-structured MoS_(2)/ZnIn_(2)S_(4) nanosheets have been prepared to capture visible light and the generated charge carriers are utilized for promoting both the oxygen reduction reaction and the oxygen evolution reaction.With the light illumination in the discharge process,the abundant photo-inspired electrons serve as the reaction sites to promote the reduction of O_(2) into LiO_(2) which is finally deposited as Li_(2)O_(2).On the contrary,the generated holes in the valence band can contribute to the low oxidization potential of Li_(2)O_(2) during the charge process.It delivers a low charge potential of 3.29 V,with an excellent resulting energy efficiency of 96.7%,much superior to that of 69.2%in the dark condition.It is noted that the involvement of photoelectrons has influenced the growth of Li_(2)O_(2) films on the MoS_(2)/ZnIn_(2)S_(4) nanosheets through the surface-adsorption pathway.The insights from the theoretical calculation confirm that the photoelectrons favor the absorption of LiO_(2) and the formation of the Li_(2)O_(2) film through the surface route.Therefore,this paper provides a deeper understanding of the mechanism of photoinspired charge carriers in LOBs and will enable further exploration of photo-involved energy storage systems.

关键词： bifunctional catalysts Li-O_(2)battery overpotential surface-route growth theoretical calculation

Design strategies of Pd-based electrocatalysts for efficient oxygen reduction

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Rare Metals 2023年第6期42卷 1778-1799页

作者： Chun-Jie Li Guang-Cun Shan Chun-Xian Guo Ru-Guang Ma School of Materials Science and Engineering Suzhou University of Science and TechnologySuzhou215009China School of Instrumentation Science and Opto-electronics Engineering Beihang UniversityBeijing100083China

Oxygen reduction reaction(ORR) occurs at the cathode of fuel cells and metal-air batteries,but usually suffers from sluggish kinetics.To solve this issue,efficient electrocatalysts are highly desired.Palladium(Pd)-based nanomaterials,as the most promising substitute of platinum(Pt),exhibit superior activity and stability in ORR electrocatalysis.The delicate regulation of the structure and/or composition shows great potential in improving the electrocatalytic ORR performance of Pd-based nanomaterials.In this review,we retrospect the recent advance of Pdbased ORR electrocatalysts,and analyses the relationship between nanostructure and catalytic performance.We start with the ORR mechanism and indicators of ORR performance in both alkaline and acidic media,followed by the synthetic methods for Pd-based nanoparticles.Then,we emphasize the design strategies of efficient Pd-based ORR catalysts from the perspective of composition,crystal phase,morphology,and support effects.Last but not least,we conclude with possible opportunities and outlook on Pd-based nanomaterials toward ORR.

关键词： Oxygen reduction reaction(ORR) Palladium(Pd) Electrocatalyst overpotential Reaction kinetics

Why do platinum catalysts show diverse electrocatalytic performance?

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Fundamental Research 2023年第5期3卷 804-808页

作者： Qiangmin Yu Zhiyuan Zhang Heming Liu Xin Kang Shiyu Ge Shaohai Li Lin Gan Bilu Liu Shenzhen Geim Graphene Center Tsinghua-Berkeley Shenzhen Institute&Institute of Materials ResearchShenzhen International Graduate SchoolTsinghua UniversityShenzhen 518055China

As one of the best electrocatalysts for the hydrogen evolution reaction,platinum catalysts are a benchmark for the performance evaluation of new catalysts.However,platinum catalysts reported in the literature show diverse electrocatalytic performances,resulting in the lack of a common reference standard.In this study,we investigated several factors that affect the performance of platinum catalysts by performing experimental measurements and data processing.These factors included the solution resistance,electrolyte temperature,loading quantity,catalyst microstructure,and normalization method of the current density.Finally,we recommended criteria for the performance evaluation of electrocatalysts.

关键词： Platinum Electrocatalyst overpotential Solution resistance Loading quantity Microstructure Catalyst area Evaluation criteria

TM-N_(2)O_(2)C_(x)单原子催化剂的设计及电催化CO_(2)还原研究

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Science China Materials 2023年第7期66卷 2741-2749页

作者：刘金杭曹小华汪锐睿陈修栋汪亚威杨平华隆加敏尹晓杰黄子健曹达鹏 School of Chemistry and Chemical Engineering Jiangxi Province Engineering Research Center of Ecological Chemical IndustryJiujiang UniversityJiujiang 332005China State Key Laboratory of Organic-Inorganic Composites Beijing University of Chemical TechnologyBeijing 100029China School of Chemistry and Material Engineering Chaohu UniversityChaohu 238000China

电催化二氧化碳还原反应(CO_(2)RR)被认为是一种潜在的碳循环技术,因为它可以利用CO_(2)作为资源在温和条件下生产高附加值燃料和化学品.因此,开发高效的二氧化碳还原反应催化剂极其重要.本文设计了一系列TM-N_(2)O_(2)C_(x)(TM=Sc,Ti,V... 详细信息

电催化二氧化碳还原反应(CO_(2)RR)被认为是一种潜在的碳循环技术,因为它可以利用CO_(2)作为资源在温和条件下生产高附加值燃料和化学品.因此,开发高效的二氧化碳还原反应催化剂极其重要.本文设计了一系列TM-N_(2)O_(2)C_(x)(TM=Sc,Ti,V,Cr,Mn,Fe,Co,Ni,Cu,Zn)单原子催化剂,并利用密度函数理论研究了其对CO_(2)RR的催化活性.这些TM-N_(2)O_(2)C_(x)催化剂在相对较低的过电位下对三种不同的产物,包括CH_(4)、CO和HCOOH,表现出优异的CO_(2)RR产品选择性,其中ScN_(2)O_(2)C_(x)、Mn-N_(2)O_(2)C_(x)、Zn-N_(2)O_(2)C_(x)的CO_(2)RR产品是CO,V-N_(2)O_(2)C_(x)的产品是CH_(4),而其他六种催化剂会产生HCOOH.此外,该研究还揭示了CH_(4)形成的最佳途径,即*+CO_(2)→C*OOH→C*O+H_(2)O→C*HO→C*HOH→C*H+H_(2)0→C*H_(2)→C*H_(3)→*+CH_(4).总之,TMN_(2)O_(2)C_(x)催化剂对电催化CO_(2)RR表现出较高的催化活性,这为实验合成这些有前景的CO_(2)RR催化剂提供了有价值的信息.

关键词： electrocatalytic CO_(2)reduction single-atom catalyst metal-N_(2)O_(2)local structure overpotential transition metal

N-heterocyclic carbene as a promising metal-free electrocatalyst with high efficiency for nitrogen reduction to ammonia

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Journal of Energy Chemistry 2020年第7期29卷 78-86,I0003页

作者： Hongyan Li Le Yang Zhongxu Wang Peng Jin Jingxiang Zhao Zhongfang Chen College of Chemistry and Chemical Engineering and Key Laboratory of Photonic and Electronic Bandgap MaterialsMinistry of EducationHarbin Normal UniversityHarbin 150025HeilongjiangChina School of Materials Science and Engineering Hebei University of TechnologyTianjin 300130China Department of Chemistry University of Puerto RicoRio Piedras CampusSan JuanPR 00931USA

Electrocatalytic nitrogen reduction reaction(NRR)at ambient conditions holds great promise for sustainably synthesizing ammonia(NH3),while developing highly-efficient,long-term stable,and inexpensive catalysts to activate the inert N≡N bond is a key scientific issue.In this work,on the basis of the concept"N-heterocyclic carbenes(NHCs)",we propose a carbon decorated graphitic-carbon nitride(C/g-C3N4)as novel metal-free NRR electrocatalyst by means of density functional theory(DFT)computations.Our results reveal that the introduced C atom in g-C3N4 surface can be regarded as NHCs and catalytic sites for activating N≡N bond,and are stabilized by the g-C3N4 substrate due to sterically disfavored dimerization.Especially,this NHCs-based heterogeneous catalysis can efficiently reduce the activated N2 molecule to NH3 with a low overpotential of 0.05 V via an enzymatic mechanism.Our work is the first report of NHCs-based electrocatalyst for N2 fixation,thus opening an alternative avenue for advancing sustainable NH3 production.

关键词： Nitrogen reduction reaction N-heterocyclic carbenes overpotential Density functional theory

Influence of process parameters on electrochemical and physical properties of sputtered iron-doped nickel oxide thin films

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Transactions of Nonferrous Metals Society of China 2006年第6期7卷 1301-1306页

作者：黄金昭徐征李海玲亢国虎王文静 Key Laboratory of Luminescence and Optical Information Ministry of EducationInstitute of Optoelectronic TechnologyBeijing Jiaotong University Beijing Solar Energy Research Institute

The iron-doped nickel oxide films used as oxygen evolution catalysts in the photoelectrochemical production of hydrogen from solar energy were deposited by means of RF reactive magnetron sputtering from a Ni-Fe alloy target in oxygen and argon atmosphere.The effects of processing parameters on the film properties,such as overpotential,composition,surface morphology and preferred orientation,were investigated.The electrochemical experiment,structural and compositional measurements indicate that the relative lower substrate temperature,higher RF power,higher working pressure and oxygen content are necessary to gain lower overpotential.The lowest overpotential of 251 mV is obtained at a current density of 80 mA/cm2.The existence of iron,which acts as activity site,and Ni3+ ion is responsible for lowering overpotential.By analyzing SEM and XRD data,it is also noticed that an improvement in crystallinity,appropriate grain size and less crystalline phase contribute to an increased electrocatalytic activity in oxygen evolution reaction.These results mentioned above indicate that iron-doped nickel oxide is promising as an oxygen catalyst.

关键词： iron-doped nickel oxide films overpotential photoelectrochemical

Environment friendly hydrothermal synthesis of carbon–Co3O4 nanorods composite as an efficient catalyst for oxygen evolution reaction

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Journal of Energy Chemistry 2017年第4期26卷 695-702页

作者： Amol R.Jadhav Harshad A.Bandal Ashif H.Tamboli Hern Kim Department of Energy Science and Technology Smart Living Innovation Technology CenterMyongji UniversityYonginGyeonggi-do 17058Republic of Korea

The design of cost-effective, highly active catalysts for hydrogen energy production is a vital element in the societal pursuit of sustainable energy. Water electrolysis is one of the most convenient processes to produce high purity hydrogen. Cobalt-based catalysts are well-known electrocatalysts for oxygen evolution reaction（OER）. In this article, all these merits indicate that the present cobalt nanocomposite is a promising electrocatalyst for OER. C–CoO-nanorods catalyst with nanorod structure was synthesized by hydrothermal treatment of CoCl·6HO/dextrose/urea mixture at 180 °C for 18 h and then calcined at400 °C for 3.5 h. The role of dextrose percentage in solution to achieve the uniform coating of carbon on the surface of CoO-nanorods has been demonstrated. The prepared materials were characterized by X-ray diffraction（XRD）, X-ray photoelectron spectrum（XPS）, field emission scanning electron microscopy（FE-SEM）, high-resolution transmission electron microscopy（HR-TEM）, and Brunauer–Emmett–Teller instrument（BET）. Due to its unique morphology, the C–CoO-nanorods catalyst exhibited better activity than CoO-microplates catalyst for OER in 1 M KOH aqueous solution. The results showed a highly efficient, scalable, and low-cost method for developing highly active and stable OER electrocatalysts in alkaline solution.

关键词： Oxygen evolution reaction overpotential Tafel slope Synergistic effect