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Total conversion of centimeter-scale nickel foam into single atom electrocatalysts with highly selective CO_(2)electrocatalytic reduction in neutral electrolyte

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Nano Research 2023年第2期16卷 2003-2010页

作者： Qikui Fan Pengfei Gao Shan Ren Yunteng Qu Chuncai Kong Jian Yang Yuen Wu Ministry of Education Key Laboratory for Non-equilibrium Synthesis and Modulation of Condensed Matter Shaanxi Province Key Laboratory of Advanced Functional Materials and Mesoscopic PhysicsSchool of PhysicsXi’an Jiaotong UniversityXi’an 710049China Shenzhen Key Laboratory of Special Functional Materials Guangdong Research Center for Interfacial Engineering of Functional MaterialsCollege of Materials Science and EngineeringShenzhen UniversityShenzhen 518060China Northwest Institute of Nuclear Technology Xi’an 710024China Institute of Functional Nano&Soft Materials(FUNSOM) Jiangsu Key Laboratory for Carbon-Based Functional Materials&DevicesSoochow UniversitySuzhou 215123China State Key Laboratory of Photoelectric Technology and Functional Materials International Collaborative Center on Photoelectric Technology and Nano Functional MaterialsInstitute of Photonics and Photon-TechnologyNorthwest UniversityXi’an 710069China Department of Chemistry iChEM(Collaborative Innovation Center of Chemistry for Energy Materials)University of Science and Technology of ChinaHefei 230026China

To improve the atomic utilization of metals and reduce the cost of industrialization,the one-step total monoatomization of macroscopic bulk metals,as opposed to nanoscale metals,is *** this study,we used a thermal diffusion method to directly convert commercial centimeter-scale Ni foam to porous Ni single-atom-loaded carbon nanotubes(CNTs).As expected,owing to the coating of single-atom on porous,highly conductive CNT carriers,Ni single-atom electrocatalysts(Ni-SACs)exhibit extremely high activity and selectivity in CO_(2)electroreduction(CO_(2)RR),yielding a current density of>350 mA/cm^(2),a selectivity for CO of>91%under a flow cell configuration using a 1 M potassium chloride(KCl)*** on the superior activity of the Ni-SACs electrocatalyst,an integrated gas-phase electrochemical zero-gap reactor was introduced to generate a significant amount of CO current for potential practical *** overall current can be increased to 800 mA,while maintaining CO Faradaic efficiencies(FEs)at above 90%per unit *** findings and insights on the active site transformation mechanism for macroscopic bulk Ni foam conversion into single atoms can inform the design of highly active single-atom catalysts used in industrial CO_(2)RR systems.

关键词： Ni single atom electrocatalyst CO_(2)electroreduction to CO neutral electrolyte thermal diffusion

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Bismuth stabilized by ZIF derivatives for electrochemical ammonia production:Proton donation effect of phosphorus dopants

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Nano Research 2023年第4期16卷 4574-4581页

作者： Qiaoling Wu Ying Sun Qin Zhao Hui Li Zhengnan Ju Yu Wang Xiaodong Sun Baohua Jia Jieshan Qiu Tianyi Ma Institute of Clean Energy Chemistry Key Laboratory for Green Synthesis and Preparative Chemistry of Advanced Materials of Liaoning ProvinceCollege of ChemistryLiaoning UniversityShenyang 110036China School of Science RMIT UniversityMelbourneVIC 3000Australia College of Chemical Engineering State Key Laboratory of Chemical Resource EngineeringBeijing University of Chemical TechnologyBeijing 100029China

N2 electroreduction reaction(NRR)offers a feasible and promising alternative for NH_(3)production by using clean energy ***,it is still obstructed by the pretty low NH3 yield rate and Faradaic efficiency(FE)primarily due to the undesired competing hydrogen evolution reaction and the extremely stable N≡N ***,bismuth nanoparticles were successfully embedded in N and P co-doped carbon nanoflakes(Bi/NPC)by high-temperature pyrolyzation of Bi-zeolitic imidazole frameworks(ZIF)followed by phosphorization,and used as a high-efficiency catalyst toward N2 electroreduction to *** 0.1 M KHCO_(3)electrolyte,Bi/NPC exhibits excellent NRR performances,including a high NH3 yield rate of 3.12μg·h^(−1)·cm^(−2)(−0.6 V *** hydrogen electrode(RHE)),an outstanding FE of 13.58%(−0.4 V ***),and a remarkable stability up to 36 h under ambient *** outstanding NRR catalytic activity is mainly attributed to the intrinsic electrocatalytic NRR activity combined with the inert hydrogen evolution reaction(HER)activity of Bi,the adsorption and activation of N2 facilitated by N dopants,as well as the superior conductivity and the large specific surface area of the two-dimensional layered carbon ***,the hydrogen source provided by P dopant promotes the hydrogenation of the adsorbed N,which further boosts the NRR performance in alkaline *** ultralong durability of Bi/NPC is attributed to the highly dispersed bismuth catalytic active centers confined in the skeleton of N and P co-doped carbon nanoflakes,which inhibits the agglomeration of bismuth *** work presents a novel avenue for designation and fabrication of high-performance Bi-based electrocatalysts for NRR.

关键词： N2 reduction bismuth N P co-doped carbon nanoflakes electrocatalysis

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Persistence of charge density wave against variation of band structures in V_(x)Ti_(1−x)Se_(2)(x=0–0.1)

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Nano Research 2024年第3期17卷 2129-2135页

作者： Zhanfeng Liu Tongrui Li Wen Zhu Hongwei Shou Mukhtar Lawan Adam Qilong Cui Yuliang Li Sheng Wang Yunbo Wu Hongen Zhu Yi Liu Shuangming Chen Xiaojun Wu Shengtao Cui Li Song Zhe Sun National Synchrotron Radiation Laboratory CAS Center for Excellence in NanoscienceUniversity of Science and Technology of ChinaHefei 230029China CAS Key Laboratory of Strongly-coupled Quantum Matter Physics University of Science and Technology of ChinaHefei 230026China Collaborative Innovation Center of Advanced Microstructures Nanjing 210093China State Key Laboratory of Inorganic Synthesis and Preparative Chemistry College of ChemistryJilin UniversityChangchun 130012China School of Chemistry and Materials Sciences CAS Key Laboratory of Materials for Energy Conversionand CAS Center for Excellence in NanoscienceUniversity of Science and Technology of ChinaHefei 230026China School Zhejiang Institute of Photonelectronics Jinhua 321004China

Charge density wave(CDW)is a phenomenon that occurs in materials,accompanied by changes in their intrinsic electronic *** study of CDW and its modulation in materials holds tremendous significance in materials research,as it provides a unique approach to controlling the electronic properties of ***_(2) is a typical layered material with a CDW phase at low *** V substitution for Ti in TiSe_(2),we tuned the carrier concentration in V_(x)Ti_(1-x)Se_(2) to study how its electronic structures ***-resolved photoemission spectroscopy(ARPES)shows that the band-folding effect is sustained with the doping level up to 10%,indicating the persistence of the CDW phase,even though the band structure is strikingly different from that of the parent compound TiSe_(2).Though CDW can induce the band fold effect with a driving force from the perspective of electronic systems,our studies suggest that this behavior could be maintained by lattice distortion of the CDW phase,even if band structures deviate from the electron-driven CDW *** work provides a constraint for understanding the CDW mechanism in TiSe_(2),and highlights the role of lattice distortion in the band-folding effect.

关键词： charge density wave band structure lattice distortion

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Bi nanoparticles encapsulated in nitrogen-doped carbon as a long-life anode material for magnesium batteries

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Journal of Magnesium and Alloys 2023年第11期11卷 4181-4188页

作者： Junjun Wang Ruohan Yu Jianxiang Wang Juncai Long Fan Qiao Lei Zhang Guanjie He Qinyou An Liqiang Mai State Key Laboratory of Advanced Technology for Materials Synthesis and Processing School of Materials Science and EngineeringWuhan University of TechnologyWuhan 430070China Christopher Ingold Laboratory Department of ChemistryUniversity College London20 Gordon StreetLondon WC1H 0AJUnited Kingdom of Great Britain and Northern IrelandUnited Kingdom Hubei Longzhong Laboratory Wuhan University of Technology(Xiangyang Demonstration Zone)Xiangyang 441000China

Bismuth has garnered significant interest as an anode material for magnesium batteries(MBs) because of its high volumetric specific capacity and low working potential. Nonetheless, the limited cycling performance(≤100 cycles) limits the practical application of Bi as anode for MBs. Therefore, the improvement of Bi cycling performance is of great significance to the development of MBs and is also full of challenges. Here, Bi nanoparticles encapsulated in nitrogen-doped carbon with single-atom Bi embedded(Bi@NC) are prepared and reported as an anode material for MBs. Bi@NC demonstrates impressive performance, with a high discharge capacity of 347.5 mAh g^(-1) and good rate capability(206.4 mAh g^(-1)@500 mA g^(-1)) in a fluoride alkyl magnesium salt electrolyte. In addition, Bi@NC exhibits exceptional long-term stability, enduring 400 cycles at 500 mA g^(-1). To the best of our knowledge, among reported Bi and Bi-based compounds for MBs, Bi@NC exhibits the longest cycle life in this work. The magnesium storage mechanism of Bi@NC is deeply studied through X-ray diffraction, transmission electron microscopy and X-ray photoelectron spectroscopy. This work provides some guidance for further improving the cycling performance of other alloy anodes in MBs.

关键词： Magnesium batteries Bismuth 3D tomography reconstruction Magnesium alloy Single-atom

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All-Climate Stretchable Dendrite-Free Zn-Ion Hybrid Supercapacitors Enabled by Hydrogel Electrolyte Engineering

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Energy & Environmental materials 2023年第2期6卷 381-388页

作者： Yuqi Jiang Kun Ma Meiling Sun Yuanyuan Li Jinping Liu State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070China The Institute of Technological Sciences Wuhan UniversityWuhan 430072China School of Chemistry Chemical Engineering and Life ScienceWuhan University of TechnologyWuhan 430070China School of Optical and Electronic Information Huazhong University of Science and TechnologyWuhan 430074China Key Laboratory for Photonic and Electronic Bandgap Materials Ministry of EducationSchool of Physics and Electronic EngineeringHarbin Normal UniversityHarbin 150025China

Hybrid supercapacitors have shown great potentials to fulfill the demand of future diverse applications such as electric vehicles and portable/wearable *** particular,aqueous zinc-ion hybrid supercapacitors(ZHSCs)have gained much attention due to their low-cost,high energy density,and environmental ***,typical ZHSCs use Zn metal anode and normal liquid electrolyte,causing the dendrite issue,restricted working temperature,and inferior device ***,a novel flexible Zn-ion hybrid supercapacitor(FZHSC)is developed by using activated carbon(AC)anode,δ-MnO_(2) cathode,and innovative PVA-based gel *** this design,heavy Zn anode and its dendrite issue are avoided and layered cathode with large interlayer spacing is *** addition,flexible electrodes are prepared and integrated with an anti-freezing,stretchable,and compressible hydrogel electrolyte,which is attained by simultaneously using glycerol additive and freezing/thawing technique to regulate the hydrogen bond and *** resulting FZHSC exhibits good rate capability,high energy density(47.86 Wh kg^(−1);3.94 mWh cm^(−3)),high power density(5.81 kW kg^(−1);480 mW cm^(−3)),and excellent cycling stability(~91%capacity retention after 30000 cycles).Furthermore,our FZHSC demonstrates outstanding flexibility with capacitance almost unchanged even after various continuous shape *** hydrogel electrolyte still maintains high ionic conductivity at ultralow temperatures(≤−30℃),enabling the FZHSC cycled well,and powering electronic timer robustly within an all-climate temperature range of−30~80℃.This work highlights that the promising Zn metal-free aqueous ZHSCs can be designed with great multifunctionality for more practical application scenarios.

关键词： all-climate operation dendrite-free anode high flexibility multifunctional gel electrolyte Zn-ion hybrid supercapacitor

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Swarming Responsive Photonic Nanorobots for Motile-Targeting Microenvironmental Mapping and Mapping-Guided Photothermal Treatment

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Nano-Micro Letters 2023年第9期15卷 205-223页

作者： Luolin Li Zheng Yu Jianfeng Liu Manyi Yang Gongpu Shi Ziqi Feng Wei Luo Huiru Ma Jianguo Guan Fangzhi Mou State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070People’s Republic of China School of Materials and Microelectronics Wuhan University of TechnologyWuhan 430070People’s Republic of China School of Materials Science and Engineering Wuhan University of TechnologyWuhan 430070People’s Republic of China School of Chemistry Chemical Engineering and Life ScienceWuhan University of TechnologyWuhan 430070People’s Republic of China

Micro/nanorobots can propel and navigate in many hard-to-reach biological environments,and thus may bring revolutionary changes to biomedical research and ***,current MNRs lack the capability to collectively perceive and report physicochemical changes in unknown *** we propose to develop swarming responsive photonic nanorobots that can map local physicochemical conditions on the fly and further guide localized photothermal *** RPNRs consist of a photonic nanochain of periodically-assembled magnetic Fe_(3)O_(4)nanoparticles encapsulated in a responsive hydrogel shell,and show multiple integrated functions,including energetic magnetically-driven swarming motions,bright stimuli-responsive structural colors,and photothermal ***,they can actively navigate in complex environments utilizing their controllable swarming motions,then visualize unknown targets(e.g.,tumor lesion)by collectively mapping out local abnormal physicochemical conditions(e.g.,pH,temperature,or glucose concentra-tion)via their responsive structural colors,and further guide external light irradiation to initiate localized photothermal *** work facilitates the development of intelligent motile nanosensors and versatile multifunctional nanotheranostics for cancer and inflam-matory diseases.

关键词： Micro/nanorobots Collective behaviors Responsive photonic crystals On-the-fly sensing Photothermal therapy

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Three-dimensional ordered hierarchically porous carbon materials for high performance Li-Se battery

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Journal of Energy Chemistry 2022年第5期31卷 624-636页

作者： Hongyan Li Wenda Dong Chao Li Tarek Barakat Minghui Sun Yingying Wang Liang Wu Lang Wang Lei Xia Zhi-Yi Hu Yu Li Bao-Lian Su Laboratory of Inorganic Materials Chemistry(CMI) University of NamurB-5000 NamurBelgium Namur Institute of Structured Matter(NISM) University of NamurB-5000 NamurBelgium State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430074HubeiChina

Developing host materials with high specific surface area, good electron conductivity, and fast ion transportation channel is critical for high performance lithium-selenium(Li-Se) batteries. Herein, a series of three dimensional ordered hierarchically porous carbon(3D OHPC) materials with micro/meso/macropores are designed and synthesized for Li-Se battery. The porous structure is tuned by following the concept of the generalized Murray’s law to facilitate the mass diffusion and reduce ion transport *** optimized 3D Se/OHPC cathode exhibits a very high 2 nd discharge capacity of 651 m Ah/g and retains 361 m Ah/g after 200 cycles at 0.2 C. Even at a high current rate of 5 C, the battery still shows a discharge capacity as high as 155 m Ah/g. The improved electrochemical performance is attributed to the synergy effect of the interconnected and well-designed micro, meso and macroporosity while shortened ions diffusion pathways of such Murray materials accelerate its ionic and electronic conductivities leading to the enhanced electrochemical reaction. The diffusivity coefficient in Se/OHPC can reach a very high value of 1.3 × 10^(-11)cm^(2)/s, much higher than those in single pore size carbon hosts. Their effective volume expansion accommodation capability and reduced dissolution of polyselenides ensure the high stability of the battery. This work, for the first time, established the clear relationship between textural properties of cathode materials and their performance and demonstrates that the concept of the generalized Murray’s law can be used as efficient guidance for the rational design and synthesis of advanced hierarchically porous materials and the great potential of 3D OHPC materials as a practical high performance cathode material for Li-Se batteries.

关键词： 3D ordered hierarchically porous carbon(OHPC) Shuttle effect Cyclability High rate capability The generalized Murray’s law Li-Se batteries

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Tunable Ru-Ru2P heterostructures with charge redistribution for efficient pH-universal hydrogen evolution

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InfoMat 2022年第5期4卷 164-173页

作者： Ding Chen Ruohan Yu Ruihu Lu Zonghua Pu Pengyan Wang Jiawei Zhu Pengxia Ji Dulan Wu Jinsong Wu Yan Zhao Zongkui Kou Jun Yu Shichun Mu State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhanChina Foshan Xianhu Laboratory of the Advanced Energy Science and Technology Guangdong Laboratory Xianhu Hydrogen ValleyFoshanChina Nanostructure Research Centre(NRC) Wuhan University of TechnologyWuhanChina State Key Laboratory of Silicate Materials for Architectures International School of Materials Science and EngineeringWuhan University of TechnologyWuhanChina

Designing synergistic heterogeneous catalytic interfaces is the key to developing highly compatible pH-universal electrocatalysts for complex chemical envi*** theoretical calculation results demonstrate that the Ru-Ru2P heterointerface can not only promote the redistribution of charges,but also reduce the d-band center,and then enhances the adsorption capacity of the key ***,in situ and facile synthesis of Ru-Ru2P heterostructures is severely limited by thermodynamic ***,we propose a molten salt-assisted catalytic synthesis scheme,and successfully build a series of homologous metallic Ru-Ru2P heterostructure catalysts with different molar ratios of Ru to P under atmospheric pressure and low-temperature(400C).The resultant Ru-Ru2P with rich heterostructures show the Pt-like HER performance in different pH ***,it is prominent under alkaline conditions(18 mV@10 mA cm^(2)),which outperforms the Pt catalyst(37 mV@10 mA cm^(2)).Furthermore,Ru-Ru2P heterostructures also show certain potential in the electrolysis of seawater to produce *** work represents a significant supplement of high-efficiency pH-universal HER catalysts,and provides a new light on interface engineering in energy technology fields and beyond.

关键词： DFT calculation heterostructure molten salt-assisted synthesis pH-universal hydrogen evolution ruthenium phosphide

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Unraveling the reaction reversibility and structure stability of nickel sulfide anodes for lithium ion batteries

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Journal of Energy Chemistry 2023年第5期80卷 392-401,I0010页

作者： Yu Huang Chunyuan Liang Yueling Cai Yi Zhou Bingkun Guo Jipeng Cheng Heguang Liu Peng Wang Qianqian Li Anmin Nie Hongtao Wang Jinsong Wu Tongyi Zhang Materials Genome Institute Shanghai UniversityShanghai 200444China Center for X-mechanics Zhejiang UniversityHangzhou 310027ZhejiangChina School of Materials Science and Engineering Zhejiang UniversityHangzhou 310027ZhejiangChina School of Materials Science and Engineering Xi'an University of TechnologyXi'an 048ShaanxChin Shanghai Key Laboratory of Mechanics in Energy Engineering Shanghai Institute of Applied Mathematics and MechanicsSchool of Mechanics and Engineering ScienceShanghai UniversityShanghai 200444China Center for High Pressure Science State Key Laboratory of Metastable Materials Science and TechnologyYanshan UniversityQinhuangdao 066004HebeiChina State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Nanostructure Research CenterWuhan University of TechnologyWuhan 430070HubeiChina

The electrochemical performance of lithium-ion batteries,*** capacity and cyclability,is primarily determined by chemical reversibility and structural stability of the electrodes in *** we have investigated the fundamental reaction behaviors of nickel sulfide(NixSy)as lithium-ion battery anodes by in-situ *** find that Ni_(3)S_(2)is the electrochemically stable phase,which appears in the first cycle of the *** the second cycle,conversion between Ni_(3)S_(2)and Li_(2)S/Ni is the dominant electrochemical *** lithiation,the NixSynanoparticles evolve into a mixture of Ni nanocrystals embedded in Li_(2)S matrix,which form a porous structure upon full lithiation,and with the recrystallization of the Ni_(3)S_(2)phase in delithiation,a compact and interconnected network is *** stability in cycles is susceptible to particle size and substrate *** substrate can certainly improve the tolerance for size-dependent pulverization of *** NixSynanoparticle exceeds the critical size value,the morphology of the particle is no longer well maintained even under the constraints of the carbon *** work deepens the understanding of electrochemical reaction behavior of conversiontype materials and helps to rational design of high-energy density battery anodes.

关键词： Nickel sulfide anodes Reaction reversility Structure rebuilding In-situ TEM Lithium-ion battery

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Advances in ultra-high temperature ceramics,composites,and coatings

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Journal of advanced Ceramics 2022年第1期11卷 1-56页

作者： Dewei NI Yuan CHENG Jiaping ZHANG Ji-Xuan LIU Ji ZOU Bowen CHEN Haoyang WU Hejun LI Shaoming DONG Jiecai HAN Xinghong ZHANG Qiangang FU Guo-Jun ZHANG State Key Laboratory of High Performance Ceramics&Superfine Microstructure Structural Ceramics and Composites Engineering Research CenterShanghai Institute of CeramicsChinese Academy of SciencesShanghai 200050China National Key Laboratory of Science and Technology on Advanced Composites in Special Environments Center for Composite Materials and StructuresHarbin Institute of TechnologyHarbin 150001China Shaanxi Key Laboratory of Fiber Reinforced Light Composite Materials Northwestern Polytechnical UniversityXi’an 710072China State Key Laboratory for Modification of Chemical Fibers and Polymer Materials Institute of Functional MaterialsDonghua UniversityShanghai 201620China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070China University of Chinese Academy of Sciences Beijing 100049China

Ultra-high temperature ceramics(UHTCs)are generally referred to the carbides,nitrides,and borides of the transition metals,with the Group IVB compounds(Zr&Hf)and TaC as the main *** UHTCs are endowed with ultra-high melting points,excellent mechanical properties,and ablation resistance at elevated *** unique combinations of properties make them promising materials for extremely environmental structural applications in rocket and hypersonic vehicles,particularly nozzles,leading edges,and engine components,*** addition to bulk UHTCs,UHTC coatings and fiber reinforced UHTC composites are extensively developed and applied to avoid the intrinsic brittleness and poor thermal shock resistance of bulk ***,high-entropy UHTCs are developed rapidly and attract a lot of attention as an emerging direction for ultra-high temperature *** review presents the state of the art of processing approaches,microstructure design and properties of UHTCs from bulk materials to composites and coatings,as well as the future directions.

关键词： ultra-high temperature ceramics(UHTCs) coatings composites high-entropy ultra-high temperature ceramics

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