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Alloy/layer double hydroxide interphasic synergy via nano-heterointerfacing for highly reversible CO_(2)redox reaction in Li-CO_(2)batteries

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Nano Research 2024年第6期17卷 5206-5215页

作者： Tianzhen Jian Wenqing Ma Jiagang Hou Jianping Ma Xianhong Li Haiyang Gao Caixia Xu Hong Liu Institute for Advanced Interdisciplinary Research(iAIR) Collaborative Innovation Center of Technology and Equipment for Biological Diagnosis and Therapy in Universities of ShandongSchool of Chemistry and Chemical EngineeringUniversity of JinanJinan 250022China Kyiv College at Qilu University of Technology Qilu University of Technology(Shandong Academy of Sciences)Jinan 250353China State Key Laboratory of Crystal Materials Shandong UniversityJinan 250100China Shandong Sacred Sun Power Sources Co. Ltd.Qufu 273100China

Li-CO_(2)batteries are among the most intriguing techniques for balancing the carbon cycle,but are challenged by the annoyed thermodynamic barrier of the Li_(2)CO_(3)decomposition reaction.Herein,we demonstrate the electrocatalytic performances of two-dimensional(2D)CoAl-layer double hydroxide(LDH)nanosheets can be significantly improved by trans-dimensional crosslinking with three-dimensional(3D)multilevel nanoporous(MP)-RuCoAl alloy(MP-RuCoAl alloy⊥CoAl-LDH).The MP-RuCoAl alloy⊥CoAl-LDH with multiscale pore channels and abundant nano-heterointerface is directly prepared by controllable etching Al from a Ru-Co-Al master alloy along with simultaneous partial oxidization of Al and Co atoms.The MP-RuCoAl is composed of various intermetallic compounds and Ru with abundant grain boundaries,and forms numerous heterointerface with 2D CoAl-LDH nanosheets.The multiscale porous metallic network benefits mass and electron transportation as well as discharge product storage and enables a rich multiphase reaction interface.In situ differential electrochemical mass spectrometry shows that the mass-to-charge ratio in the charging process is~0.733 which is consistent with the theoretical value of 3/4,stating that the reversible co-decomposition of Li_(2)CO_(3)and C can be achieved with the MP-RuCoAl alloy⊥CoAl-LDH.The Ketjen black(KB)/MP-RuCoAl⊥CoAl-LDH battery demonstrates a high cyclability for over 2270 h(227 cycles)with a lower voltage gap stabilized at~1.3 V at 200 mA·g^(−1).Our findings here provide useful guidelines for developing high efficiency transition metal based electrocatalysts by coupling with conductive porous substrate for impelling the development of practical Li-CO_(2)battery systems.

关键词： heterojunction interface nanoporous Li-CO_(2)battery dealloying

Dynamic surface restructuring of nanoporous Cu_(2-x)Se for efficient CO_(2) electroreduction into methanol

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Journal of Energy Chemistry 2022年第8期31卷 514-520,I0014页

作者： Xin Lin Xunlin Liu Yang Zhao Jiao Lan Kang Jiang Zhixiao Liu Feng Xie Yongwen Tan College of Materials Science and Engineering State Key Laboratory of Advanced Design and Manufacturing for Vehicle BodyHunan UniversityChangsha 410082HunanChina College of Materials Science and Engineering Hunan UniversityChangsha 410082HunanChina

The nanoporous Cu_(2-x)Se with Cu(Se-5%)surface catalysts were prepared through in situ dynamic restructuring strategy during the electrochemical process,which achieves highly selective electrochemical CO_(2) reduction to methanol.In situ and quasi-operando spectroscopic results provide a deep insight into the catalytic active centres of reconstructed heterogeneous catalysts for CO_(2) electroreduction.

关键词： Surface restructuring nanoporous Cu_(2-x)Se Carbon dioxide reduction Methanol

Point-defect engineering of nanoporous CuBi_(2)O_(4) photocathode via rapid thermal processing for enhanced photoelectrochemical activity

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Journal of Energy Chemistry 2022年第8期31卷 201-209,I0007页

作者： Li Qu Runfa Tan Arumugam Sivanantham Min Je Kang Yoo Jae Jeong Dong Hyun Seo Sungkyu Kim In Sun Cho Department of Materials Science&Engineering Ajou UniversitySuwon 16499South Korea Department of Energy Systems Research Ajou UniversitySuwon 16499South Korea Department of Nanotechnology and Advanced Materials Engineering Sejong UniversitySeoul 05006South Korea

Engineering point defects such as metal and oxygen vacancies play a crucial role in manipulating the electrical,optical,and catalytic properties of oxide semiconductors for solar water splitting.Herein,we synthesized nanoporous CuBi_(2)O_(4)(np-CBO)photocathodes and engineered their surface point defects via rapid thermal processing(RTP)in controlled atmospheres(O_(2),N_(2),and vacuum).We found that the O_(2)-RTP treatment of np-CBO increased the charge carrier density effectively without hampering the nanoporous morphology,which was attributed to the formation of copper vacancies(VCu).Further analyses revealed that the amounts of oxygen vacancies(Vo)and Cu^(1+)were reduced simultaneously,and the relative electrochemical active surface area increased after the O_(2)-RTP treatment.Notably,the point defects(VC_(u),Cu^(1+),and Vo)regulated np-CBO achieved a superb water-splitting photocurrent density of-1.81 m A cm^(-2) under simulated sunlight illumination,which is attributed to the enhanced charge transport and transfer properties resulting from the regulated surface point defects.Finally,the reversibility of the formation of the point defects was checked by sequential RTP treatments(O_(2)-N_(2)-O_(2)-N_(2)),demonstrating the strong dependence of photocurrent response on the RTP cycles.Conclusively,the surface point defect engineering via RTP treatment in a controlled atmosphere is a rapid and facile strategy to promote charge transport and transfer properties of photoelectrodes for efficient solar water-splitting.

关键词： nanoporous Copper bismuth oxide Rapid thermal processing Copper vacancy Charge transport

Intermetallic-driven highly reversible electrocatalysis in Li–CO_(2) battery over nanoporous Ni_(3)Al/Ni heterostructure

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eScience 2023年第3期3卷 79-88页

作者： Tianzhen Jian Wenqing Ma Caixia Xu Hong Liu John Wang Institute for Advanced Interdisciplinary Research(iAIR) School of Chemistry and Chemical EngineeringCollaborative Innovation Center of Technology and Equipment for Biological Diagnosis and Therapy in Universities of ShandongUniversity of JinanJinan250022China Department of Materials Science and Engineering National University of SingaporeSingapore117574Singapore Institute of Materials Research and Engineering A*StarSingapore138634Singapore

Li–CO_(2) batteries,which integrate CO_(2) utilization and electrochemical energy storage,offer the prospect of utilizing a greenhouse gas and providing an alternative to the well-established lithium-ion batteries.However,they still suffer from rather limited reversibility,low energy efficiency,and sluggish CO_(2) redox reaction kinetics.To address these key issues,a nanoporous Ni_(3)Al intermetallic/Ni heterojunction(NP–Ni_(3) Al/Ni)is purposely engi-neered here via an alloying–etching protocol,whereby the unique interactions between Al and Ni in Ni_(3)Al endow NP-Ni_(3)Al/Ni with optimum reactant/product adsorption and thus unique catalytic performance for the CO_(2) redox reaction.Furthermore,the nanoporous spongy structure benefits mass transport as well as discharge product storage and enables a rich multiphase reaction interface.In situ Raman studies and theoretical simulations reveal that both CO_(2) reduction and the co-decomposition of Li_(2)CO_(3) and C are distinctly promoted by NP-Ni_(3)Al/Ni,thereby greatly improving catalytic activity and stability.NP-Ni_(3)Al/Ni offers promising application potential in Li–CO_(2) batteries,with its scalable fabrication,low production cost,and superior catalytic performance.

关键词： Ni_(3)Al intermetallic nanoporous Li-CO_(2)batteries Dealloying

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nanoporous magnesium

Nano Research 2018年第12期11卷 6428-6435页

作者： Ilya Vladimirovich Okulov Sviatlana V.Lamaka Takeshi Wada Kunio Yubuta Mikhail L.Zheludkevich Jorg Weissmuller Jurgen Markmann Hidemi Kato Institute for Materials Research Tohoku UniversityKatahira 2-1-1Sendai980-8577Japan Institute of Materials Research Materials MechanicsHelmholtz-Zentrum Geesthacht21502GeesthachtGermany MagiC-Magnesium Innovation Centre Helmholtz-Zentrum Geesthacht21502GeesthachtGermany Faculty of Engineering University of Kiel24118KielGermany Institute of Materials Physics and Technology Hamburg University of Technology21073HamburgGermany

In this study, we present freestanding nanoporous magnesium as a novel lightweight material with high potential for structural and functional applications. Thus far, the high reactivity of Mg with oxygen and aqueous media prevented the fabrication of nanoporous Mg. First, in order to synthesize nanoporous Mg, we fabricated a bicontinuous nanocomposite consisting of interpenetrating Mg and non-Mg phases by liquid metal dealloying. The non-Mg phases in the nanocomposite protect Mg against corrosion. Second, we etched the non-Mg phases from the nanocomposite, leaving nanoporous Mg, using HF solution. This process is advantageous because the nanoporous Mg was passivated by a MgF2 layer during the etching. Our approach is very flexible, and we demonstrate that versatile microstructures of the nanoporous Mg—e.g., nanoscale bicontinuous network, hierarchical, or plate-like structures—can be designed for the given needs. More importantly, these nanoporous Mg samples can readily be exposed to air without being harmed by corrosion.

关键词： dealloying nanoporous magnesium

Surface effects on mechanical behavior of elastic nanoporous materials under high strain

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Applied Mathematics and Mechanics(English Edition) 2015年第7期36卷 927-938页

作者： Zixing LU Fan XIE Qiang LIU Zhenyu YANG School of Aeronautics Science and Engineering Beihang University

This paper studies surface effects on the mechanical behavior of nanoporous materials under high strains with an improved anisotropic Kelvin model. The stress-strain relations are derived by the theories of Euler-Bernoulli beam and surface elasticity. Mean- while, the influence of strut （or ligament） size on the mechanical properties of nanoporous materials is discussed, which becomes a key factor with consideration of the residual sur- face stress and the surface elasticity. The results show that the decrease in the strut diameter and the increase in the residual surface stress or the surface elasticity can both lead to an increase in the carrying capacity of nanoporous materials. F^lrthermore, me- chanical behaviors of anisotropic nanoporous materials in different directions （the rise direction and the transverse direction） are investigated. The results indicate that the sur- face effects in the transverse direction are more obvious than those in the rise direction for anisotropic nanoporous materials. In addition, the present results can be reduced to the cases of conventional foams as the strut size increases to micron-scale, which confirms validity of the model to a certain extent.

关键词： surface effect nanoporous anisotropy high strain

Highly efficient nanoporous CoBP electrocatalyst for hydrogen evolution reaction

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Rare Metals 2021年第5期40卷 1031-1039页

作者： Hui-Lan Guang Sheng-Li Zhu Yan-Qin Liang Shui-Lin Wu Zhao-Yang Li Shui-Yuan Luo Zhen-Duo Cui Akihisa Inoue School of Materials Science and Engineering Tianjin UniversityTianjin 300350China School of Materials Science and Engineering Lanzhou Jiaotong UniversityLanzhou 730070China College of Chemistry Engineering and Materials Science Quanzhou Normal UniversityQuanzhou 362000China International Institute of Green Materials Josai International UniversityTogane 283-8555Japan Department of Physics King Abdulaziz UniversityJeddah 22254Saudi Arabia

Water splitting is an environment friendly and efficient way to produce hydrogen.Highly efficient and low-cost non-noble metal catalysts play an important role in hydrogen evolution reaction(HER).Dealloying is a simple method to prepare three-dimensional self-supporting nanoporous materials without conductive supports and binders.In this work,we prepared self-supporting nanoporous CoBP electrocatalyst by dealloying method.The influence of the synergistic effect of nonmetallic elements on catalytic activity was investigated.The synergistic electronic effect of Co,B and P atoms on the surface optimizes the H atoms desorption and results in superior HER activity.The bi-continuous structure of nanoporous CoBP provides more active area and favors of electron and electrolyte transfer.The nanoporous CoBP with the B/P atomic ratio of 1/3 exhibits low overpotential of 42 mV at 10 mA·cm^(-2),small Tafel slope of 39.8 mV·dec-1 and good long-term stability with no performance decrease for 20 h in alkaline solution.

关键词： Hydrogen evolution reaction nanoporous Self-supporting electrocatalyst Co-B-P alloy Dealloying

Facile synthesis of nanoporous CuS nanospheres for high-performance supercapacitor electrodes

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Journal of Energy Chemistry 2017年第4期26卷 762-767页

作者： Hamid Heydari Seyyed Ebrahim Moosavifard Mohammad Shahraki Saeed Elyasi Faculty of Sciences Razi UniversityKermanshahIran Young Researchers and Elite Club Central Tehran BranchIslamic Azad UniversityTehranIran Department of Chemistry University of Sistan and BaluchestanZahedanIran Department of Chemical Engineering Sharif University of TechnologyTehranIran

In recent years, development of high-performance supercapacitor electrode materials has stimulated a great deal of scientific research. The electrochemical performance of a supercapacitor strongly depends on its material structures. Herein, we report a simple strategy for high-performance supercapacitors by building pseudocapacitive CuS nanospheres with nanoporous structures, nanosized walls（nanoporous CuS nanospheres electrode has been attributed to its unique structures that plays a key role in providing short ion and electron diffusion pathways, facilitated ion transport and more active sites for electrochemical reactions. This work sheds a new light on the metal sulfides design philosophy, and demonstrates that nanoporous CuS nanospheres electrode is a promising candidate for application in high-performance supercapacitors.

关键词： Supercapacitor nanoporous CuS Nanospheres

Adsorption characteristics of copper ion on nanoporous silica

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Acta Geochimica 2019年第4期38卷 517-529页

作者： Yanhui Niu Wenbin Yu Zonghua Qin Xin Nie Shuguang Yang Quan Wan State Key Laboratory of Ore Deposit Geochemistry Institute of GeochemistryChinese Academy of Sciences99 Lincheng West RoadGuanshanhu DistrictGuiyang 550081GuizhouChina University of Chinese Academy of Sciences Beijing 100049China School of Chemistry and Materials Science Guizhou Education University115 Gaoxin RoadWudang DistrictGuiyang 550018GuizhouChina CAS Center for Excellence in Comparative Planetology Hefei 230026AnhuiChina

Adsorption by nanoporous media is critically involved in many fundamental geological and geochemical processes including chemical weathering,element migration and enrichment,environmental pollution,etc.Yet,the adsorption behavior of metal ions on nanoporous materials has not been systematically investigated.In this study,MCM-41 material with a monodisperse pore size(4.4 nm)and a large BET specific surface area(839 m^2/g)was hydrothermally prepared and used as a model silica adsorbent to study the adsorption characteristics of Cu^2+as a representative metal ion.The Cu^2+adsorption capacity was found to increase with increasing suspension pH in the range from 3 to 5 and to decrease in the presence of NaNO3.At 25℃,pH=5,and a solid-to-liquid ratio of 5 g/L,the adsorption capacity was determined to be 0.29 mg/g,which can be converted to a dimensionless partition coefficient of 45,indicating a strong enriching effect of nanoporous silica.The adsorption isotherm and kinetic data were fitted to several commonly used thermodynamic,kinetic,and diffusion models.The adsorption mechanism was also studied by Fourier transform infrared spectroscopy,X-ray photoelectron spectroscopy and synchrotron-based X-ray absorption spectroscopy.The results suggest that Cu2+ion adsorption is an entropy-driven endothermal process,possibly involving both outer-sphere and inner-sphere complexes.

关键词： nanoporous silica Copper ion Adsorption