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Surface engineering of P2-type cathode material targeting long-cycling and high-rate sodium-ion batteries
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作者 Jun Xiao Yang Xiao +11 位作者 Shijian Wang Zefu Huang Jiayi Li Cheng Gong Guilai Zhang Bing Sun Hong Gao Huiqiao Li Xin Guo Yong Wang Hao Liu Guoxiu Wang 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第10期444-452,I0009,共10页
The widespread interest in layered P2-type Mn-based cathode materials for sodium-ion batteries(SIBs)stems from their cost-effectiveness and abundant resources.However,the inferior cycle stability and mediocre rate per... The widespread interest in layered P2-type Mn-based cathode materials for sodium-ion batteries(SIBs)stems from their cost-effectiveness and abundant resources.However,the inferior cycle stability and mediocre rate performance impede their further development in practical applications.Herein,we devised a wet chemical precipitation method to deposit an amorphous aluminum phosphate(AlPO_(4),denoted as AP)protective layer onto the surface of P2-type Na_(0.55)Ni_(0.1)Co_(0.7)Mn_(0.8)O_(2)(NCM@AP).The resulting NCM@5AP electrode,with a 5 wt%coating,exhibits extended cycle life(capacity retention of78.4%after 200 cycles at 100 mA g^(-1))and superior rate performance(98 mA h g^(-1)at 500 mA g^(-1))compared to pristine NCM.Moreover,our investigation provides comprehensive insights into the phase stability and active Na^(+)ion kinetics in the NCM@5AP composite electrode,shedding light on the underlying mechanisms responsible for the enhanced performance observed in the coated electrode. 展开更多
关键词 Layered metal oxides Sodium-ion batteries P2-type structure surface engineering
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Enhanced structural stability and durability in lithium-rich manganese-based oxide via surface double-coupling engineering
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作者 Jiayu Zhao Yuefeng Su +10 位作者 Jinyang Dong Xi Wang Yun Lu Ning Li Qing Huang Jianan Hao Yujia Wu Bin Zhang Qiongqiong Qi Feng Wu Lai Chen 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第11期274-283,共10页
Lithium-rich manganese-based oxides(LRMOs) exhibit high theoretical energy densities, making them a prominent class of cathode materials for lithium-ion batteries. However, the performance of these layered cathodes of... Lithium-rich manganese-based oxides(LRMOs) exhibit high theoretical energy densities, making them a prominent class of cathode materials for lithium-ion batteries. However, the performance of these layered cathodes often declines because of capacity fading during cycling. This decline is primarily attributed to anisotropic lattice strain and oxygen release from cathode surfaces. Given notable structural transformations, complex redox reactions, and detrimental interface side reactions in LRMOs, the development of a single modification approach that addresses bulk and surface issues is challenging. Therefore,this study introduces a surface double-coupling engineering strategy that mitigates bulk strain and reduces surface side reactions. The internal spinel-like phase coating layer, featuring threedimensional(3D) lithium-ion diffusion channels, effectively blocks oxygen release from the cathode surface and mitigates lattice strain. In addition, the external Li_(3)PO_(4) coating layer, noted for its superior corrosion resistance, enhances the interfacial lithium transport and inhibits the dissolution of surface transition metals. Notably, the spinel phase, as excellent interlayer, securely anchors Li_(3)PO_(4) to the bulk lattice and suppresses oxygen release from lattices. Consequently, these modifications considerably boost structural stability and durability, achieving an impressive capacity retention of 83.4% and a minimal voltage decay of 1.49 m V per cycle after 150 cycles at 1 C. These findings provide crucial mechanistic insights into the role of surface modifications and guide the development of high-capacity cathodes with enhanced cyclability. 展开更多
关键词 Lithium-ion battery Layered lithium-rich cathode surface double-coupling engineering Lattice strain Oxygen release
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Rational surface charge engineering of haloalkane dehalogenase for boosting the enzymatic performance in organic solvent solutions
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作者 Yin Wu Yan Sun 《Chinese Journal of Chemical Engineering》 SCIE EI CAS CSCD 2024年第1期276-285,共10页
Biocatalysis in organic solvents(OSs)has numerous important applications,but native enzymes in OSs often exhibit limited catalytic performance.Herein,we proposed a computation-aided surface charge engineering strategy... Biocatalysis in organic solvents(OSs)has numerous important applications,but native enzymes in OSs often exhibit limited catalytic performance.Herein,we proposed a computation-aided surface charge engineering strategy to improve the catalytic performance of haloalkane dehalogenase DhaA in OSs based on the energetic analysis of substrate binding to the DhaA surface.Several variants with enhanced OS resistance were obtained by replacing negative charged residues on the surface with positive charged residue(Arg).Particularly,a four-substitution variant E16R/E93R/E121R/E257R exhibited the best catalytic performance(five-fold improvement in OS resistance and seven-fold half-life increase in 40%(vol)dimethylsulfoxide).As a result,the overall catalytic performance of the variant could be at least 26 times higher than the wild-type DhaA.Fluorescence spectroscopy and molecular dynamics simulation studies revealed that the residue substitution mainly enhanced OS resistance from four aspects:(a)improved the overall structural stability,(b)increased the hydrophobicity of the local microenvironment around the catalytic triad,(c)enriched the hydrophobic substrate around the enzyme molecule,and(d)lowered the contact frequency between OS molecules and the catalytic triad.Our findings validate that computationaided surface charge engineering is an effective and ingenious rational strategy for tailoring enzyme performance in OSs. 展开更多
关键词 surface charge engineering Organic solvent resistance Molecular dynamics simulation Haloalkane dehalogenase
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Electrochemical Carbon Dioxide Reduction to Ethylene:From Mechanistic Understanding to Catalyst Surface Engineering 被引量:4
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作者 Junpeng Qu Xianjun Cao +7 位作者 Li Gao Jiayi Li Lu Li Yuhan Xie Yufei Zhao Jinqiang Zhang Minghong Wu Hao Liu 《Nano-Micro Letters》 SCIE EI CAS CSCD 2023年第10期382-415,共34页
Electrochemical carbon dioxide reduction reaction(CO_(2)RR)provides a promising way to convert CO_(2)to chemicals.The multicarbon(C_(2+))products,especially ethylene,are of great interest due to their versatile indust... Electrochemical carbon dioxide reduction reaction(CO_(2)RR)provides a promising way to convert CO_(2)to chemicals.The multicarbon(C_(2+))products,especially ethylene,are of great interest due to their versatile industrial applications.However,selectively reducing CO_(2)to ethylene is still challenging as the additional energy required for the C–C coupling step results in large overpotential and many competing products.Nonetheless,mechanistic understanding of the key steps and preferred reaction pathways/conditions,as well as rational design of novel catalysts for ethylene production have been regarded as promising approaches to achieving the highly efficient and selective CO_(2)RR.In this review,we first illustrate the key steps for CO_(2)RR to ethylene(e.g.,CO_(2)adsorption/activation,formation of~*CO intermediate,C–C coupling step),offering mechanistic understanding of CO_(2)RR conversion to ethylene.Then the alternative reaction pathways and conditions for the formation of ethylene and competitive products(C_1 and other C_(2+)products)are investigated,guiding the further design and development of preferred conditions for ethylene generation.Engineering strategies of Cu-based catalysts for CO_(2)RR-ethylene are further summarized,and the correlations of reaction mechanism/pathways,engineering strategies and selectivity are elaborated.Finally,major challenges and perspectives in the research area of CO_(2)RR are proposed for future development and practical applications. 展开更多
关键词 Key steps in CO_(2)RR-ethylene Preferable reaction pathways Mechanism understanding surface engineering strategies of Cu-based catalysts
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Selective sulfur conversion with surface engineering of electrocatalysts in a lithium-sulfur battery 被引量:2
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作者 Yuejin Zhu Yinze Zuo +4 位作者 Xuechao Jiao Revanasiddappa Manjunatha Ejikeme Raphael Ezeigwe Wei Yan Jiujun Zhang 《Carbon Energy》 SCIE CSCD 2023年第2期72-84,共13页
The sluggish kinetics of multiphase sulfur conversion with homogeneous and heterogeneous electrochemical processes,causing the“shuttle effect”of soluble polysulfide species(PSs),is the challenges in terms of lithium... The sluggish kinetics of multiphase sulfur conversion with homogeneous and heterogeneous electrochemical processes,causing the“shuttle effect”of soluble polysulfide species(PSs),is the challenges in terms of lithium-sulfur batteries(LSBs).In this paper,a Mn_(3)O_(4-x) catalyst,which has much higher activity for heterogeneous reactions than for homogeneous reactions(namely,preferentialactivity catalysts),is designed by surface engineering with rational oxygen vacancies.Due to the rational design of the electronic structure,the Mn_(3)O_(4-x) catalyst prefers to accelerate the conversion of Li2S4 into Li_(2)S_(2)/Li_(2)S and optimize Li_(2)S deposition,reducing the accumulation of PSs and thus suppressing the“shuttle effect.”Both density functional theory calculations and in situ X-ray diffraction measurements are used to probe the catalytic mechanism and identify the reaction intermediates of MnS and Li_(y)Mn_(z)O_(4-x) for fundamental understanding.The cell with Mn_(3)O_(4-x) delivers an ultralow attenuation rate of 0.028% per cycle over 2000 cycles at 2.5 C.Even with sulfur loadings of 4.93 and 7.10mg cm^(-2) in a lean electrolyte(8.4μL mg s^(-1)),the cell still shows an initial areal capacity of 7.3mAh cm^(-2).This study may provide a new way to develop preferential-activity heterogeneous-reaction catalysts to suppress the“shuttle effect”of the soluble PSs generated during the redox process of LSBs. 展开更多
关键词 electrochemical kinetics heterogeneous catalysis lithium-sulfur batteries Mn3O4-x-catalyzed separator surface engineering
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Boosting the Performance Gain of Ru/C for Hydrogen Evolution Reaction Via Surface Engineering 被引量:1
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作者 Xiaobing Bao Yuzhuo Chen +3 位作者 Shanjun Mao Yong Wang Yong Yang Yutong Gong 《Energy & Environmental Materials》 SCIE EI CAS CSCD 2023年第5期415-424,共10页
The surface properties of catalysts determine the intrinsic activity and adaptability.Ruthenium is regarded as a potential candidate to substitute platinum for water electrolysis due to the low cost and analogous elec... The surface properties of catalysts determine the intrinsic activity and adaptability.Ruthenium is regarded as a potential candidate to substitute platinum for water electrolysis due to the low cost and analogous electronic structures while it suffers from severe dissolution and stability problems.Herein,the modification of Ru/C with atomically dispersed cobalt atoms is achieved via a simple thermal doping method.The newly formed amorphous shell with Ru-Co sites on the Ru/C catalyst improved the hydrogen evolution reaction activity and stability significantly.Impressively,the obtained Co1Ru@Ru/CN_(x)catalyst exhibited an overpotential as low as 30 mV at 10 mA cm^(-2)in an alkaline medium,which is among the best HER catalysts reported so far.The oxygen oxophile Co prevents the fast oxidation and dissolution of Ru species,ensuring outstanding long-term durability up to 70 h.Theoretical calculations reveal that the Ru-Co coordination acts as a more active site for water dissociation than the Ru-Ru.Meanwhile,the"Ru-Co shell/Ru core"structures show high adaptability for the reaction conditions.This simple doping strategy offers prospects for scalable preparation of highly active electrocatalysts. 展开更多
关键词 high performance hydrogen evolution reaction ruthenium catalyst surface engineering
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Attapulgite nanorods assisted surface engineering for separator to achieve high-performance lithium–sulfur batteries 被引量:4
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作者 Wenhao Sun Xiaogang Sun +5 位作者 Naseem Akhtar Chengming Li Weikun Wang Anbang Wang Kai Wang Yaqin Huang 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2020年第9期364-374,I0011,共12页
Lithium-sulfur(Li-S)batteries have been recognized as one of the most promising candidates for nextgeneration portable electronic devices,owing to their extremely high energy density and low cost.However,the dissoluti... Lithium-sulfur(Li-S)batteries have been recognized as one of the most promising candidates for nextgeneration portable electronic devices,owing to their extremely high energy density and low cost.However,the dissolution of lithium polysulfides(LiPSs)and consequent"shuttle effect"seriously hinder the practical deployment of Li-S batteries.Herein,multi-metal oxide nanorods named attapulgite are proposed as multifunctional ionic sieve to immobilize LiPSs and further promote the regulation of LiPSs.Attapulgite,consisting of Al,Mg,Fe,Si and O ions,possesses more polar sites to immobilize LiPSs in comparison with single metal oxides.In addition,the catalytic nature(Fe ions)of attapulgite avails the LiPSs conversion reaction,which is further confirmed by the linear sweep voltammetry and electrochemical impedance spectroscopy.Benefited from the synergistic effect of multi-metal oxide and conductive carbon,the Li-S battery with the modified separator delivers remarkable discharge capacities of 1059.4 mAh g-1 and 792.5 mAh g-1 for the first and 200th cycle at 0.5 C,respectively.The work presents an effective way to improve the electrochemical performance of Li-S batteries by employing attapulgite nanorods assisted separator surface engineering. 展开更多
关键词 surface engineering Multi-metal oxide SEPARATOR Shuttle effect Synergistic effect
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Surface/interface engineering of high-efficiency noble metal-free electrocatalysts for energy-related electrochemical reactions 被引量:8
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作者 Hui Zhao Zhong-Yong Yuan 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2021年第3期89-104,共16页
To date,much efforts have been devoted to the high-efficiency noble metal-free electrocatalysts for hydrogen-and oxygen-involving energy conversion reactions,due to their abundance,low cost and nultifunctionally.Surfa... To date,much efforts have been devoted to the high-efficiency noble metal-free electrocatalysts for hydrogen-and oxygen-involving energy conversion reactions,due to their abundance,low cost and nultifunctionally.Surface/interface engineering is found to be effective in achieving novel physicochemical properties and synergistic effects in nanomaterials for electrocatalysis.Among various engineering strategies,heteroatom-doping has been regarded as a most promising method to improve the electrocatalytic performance via the regulation of electronic structure of catalysts,and numerous works were reported on the synthesis method and mechanism investigation of heteroatom-doping electrocatalysts,though the heteroatom-doping can only provide limited active sites.Engineering of other defects such as vacancies and edge sites and construction of heterostructure have shown to open up a potential avenue for the development of noble metal-free electrocatalysts.In addition,surface functionalization can attach various molecules onto the surface of materials to easily modify their physical or chemical properties,being as a promising complement or substitute for offering materials with catalytic properties.This paper gives the insights into the diverse strategies of surface/interface engineering of the highefficiency noble metal-free electrocatalysts for energy-related electrochemical reactions.The significant advances are summarized.The unique advantages and mechanisms for specific applications are highlighted.The current challenges and outlook of this growing field are also discussed. 展开更多
关键词 Noble metal-free electrocatalysts Electrocatalysis surface/interface engineering Metal-air battery Overall water splitting
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Atomic-level insights into surface engineering of semiconductors for photocatalytic CO_(2) reduction 被引量:3
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作者 Hengming Huang Hui Song +2 位作者 Jiahui Kou Chunhua Lu Jinhua Ye 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2022年第4期309-341,共33页
Photocatalytic conversion of CO_(2)into solar fuels provides a bright route for the green and sustainable development of human society.However,the realization of efficient photocatalytic CO_(2)reduction reaction(CO_(2... Photocatalytic conversion of CO_(2)into solar fuels provides a bright route for the green and sustainable development of human society.However,the realization of efficient photocatalytic CO_(2)reduction reaction(CO_(2)RR)is still challenging owing to the sluggish kinetics or unfavorable thermodynamics for basic chemical processes of CO_(2)RR,such as adsorption,activation,conversion and product desorption.To overcome these shortcomings,recent works have demonstrated that surface engineering of semiconductors,such as introducing surface vacancy,surface doping,and cocatalyst loading,serves as effective or promising strategies for improved photocatalytic CO_(2)RR with high activity and selectivity.The essential reason lies in the activation and reaction pathways can be optimized and regulated through the reconstruction of surface atomic and electronic structures.Herein,in this review,we focus on recent research advances about rational design of semiconductor surface for photocatalytic CO_(2)RR.The surface engineering strategies for improved CO_(2)adsorption,activation,and product selectivity will be reviewed.In addition,theoretical calculations along with in situ characterization techniques will be in the spotlight to clarify the kinetics and thermodynamics of the reaction process.The aim of this review is to provide deep understanding and rational guidance on the design of semiconductors for photocatalytic CO_(2)RR. 展开更多
关键词 CO_(2)reduction PHOTOCATALYSIS surface engineering Activation SELECTIVITY
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METHOD TO EXTRACT BLEND SURFACE FEATURE IN REVERSE ENGINEERING 被引量:5
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作者 LUeZhen KeYinglin +2 位作者 SunQing KelvinW HuangXiaoping 《Chinese Journal of Mechanical Engineering》 SCIE EI CAS CSCD 2003年第3期248-251,263,共5页
A new method of extraction of blend surface feature is presented. It contains two steps: segmentation and recovery of parametric representation of the blend. The segmentation separates the points in the blend region f... A new method of extraction of blend surface feature is presented. It contains two steps: segmentation and recovery of parametric representation of the blend. The segmentation separates the points in the blend region from the rest of the input point cloud with the processes of sampling point data, estimation of local surface curvature properties and comparison of maximum curvature values. The recovery of parametric representation generates a set of profile curves by marching throughout the blend and fitting cylinders. Compared with the existing approaches of blend surface feature extraction, the proposed method reduces the requirement of user interaction and is capable of extracting blend surface with either constant radius or variable radius. Application examples are presented to verify the proposed method. 展开更多
关键词 Reverse engineering Segmentation Blend surface Feature extraction
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Awakening the oxygen evolution activity of MoS_(2) by oxophilic-metal induced surface reorganization engineering 被引量:1
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作者 Xueqin Mu Yang Zhu +7 位作者 Xiangyao Gu Shipeng Dai Qixin Mao Lintao Bao Wenxuan Li Suli Liu Jianchun Bao Shichun Mu 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2021年第11期546-551,I0013,共7页
Although molybdenum disulfide (MoS_(2))-based materials are generally known as active electrocatalysts for the hydrogen evolution reaction (HER), the inert performance for the oxygen evolution reaction (OER) seriously... Although molybdenum disulfide (MoS_(2))-based materials are generally known as active electrocatalysts for the hydrogen evolution reaction (HER), the inert performance for the oxygen evolution reaction (OER) seriously limits their wide applications in alkaline electrolyzers due to there exists too strong metal-sulfur (M−S) bond in MoS_(2). Herein, by means of surface reorganization engineering of bimetal Al, Co-doped MoS_(2) (devoted as AlCo_(3)-MoS_(2)) through in situ substituting partial oxidation, we successfully significantly activate the OER activity of MoS_(2), which affords a considerably low overpotential of 323 mV at −30 mA cm^(−2), far lower than those of MoS_(2), Al-MoS_(2) and Co-MoS_(2) catalysts. Essentially, the AlCo_(3)-MoS_(2) substrate produces lots of M−O (M=Al, Co and Mo) species with oxygen vacancies, which trigger the surface self-reconstruction of pre-catalysts and simultaneously boost the electrocatalytic OER activity. Moreover, benefiting from the moderate M−O species formed on the surface, the redistribution of surface electron states is induced, thus optimizing the adsorption of OH* and OOH* intermediates on metal oxyhydroxides and awakening the OER activity of MoS_(2). 展开更多
关键词 surface reorganization engineering Porous nanosheets Oxygen evolution reaction MoS_(2) Oxophilic-metal
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Engineering homotype heterojunctions in hard carbon to induce stable solid electrolyte interfaces for sodium-ion batteries 被引量:5
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作者 Chengxin Yu Yu Li +6 位作者 Haixia Ren Ji Qian Shuo Wang Xin Feng Mingquan Liu Ying Bai Chuan Wu 《Carbon Energy》 SCIE CAS CSCD 2023年第1期181-193,共13页
Developing effective strategies to improve the initial Coulombic efficiency(ICE)and cycling stability of hard carbon(HC)anodes for sodium-ion batteries is the key to promoting the commercial application of HC.In this ... Developing effective strategies to improve the initial Coulombic efficiency(ICE)and cycling stability of hard carbon(HC)anodes for sodium-ion batteries is the key to promoting the commercial application of HC.In this paper,homotype heterojunctions are designed on HC to induce the generation of stable solid electrolyte interfaces,which can effectively increase the ICE of HC from 64.7%to 81.1%.The results show that using a simple surface engineering strategy to construct a homotypic amorphous Al_(2)O_(3) layer on the HC could shield the active sites,and further inhibit electrolyte decomposition and side effects occurrence.Particularly,due to the suppression of continuous decomposition of NaPF 6 in ester-based electrolytes,the accumulation of NaF could be reduced,leading to the formation of thinner and denser solid electrolyte interface films and a decrease in the interface resistance.The HC anode can not only improve the ICE but elevate its sodium storage performance based on this homotype heterojunction composed of HC and Al_(2)O_(3).The optimized HC anode exhibits an outstanding reversible capacity of 321.5mAhg^(−1) at 50mAg^(−1).The cycling stability is also improved effectively,and the capacity retention rate is 86.9%after 2000 cycles at 1Ag^(−1) while that of the untreated HC is only 52.6%.More importantly,the improved sodium storage behaviors are explained by electrochemical kinetic analysis. 展开更多
关键词 hard carbon anodes homotype heterojunctions sodium-ion batteries solid electrolyte interface surface engineering
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Improving the activity and stability of Ni-based electrodes for solid oxide cells through surface engineering:Recent progress and future perspectives 被引量:4
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作者 Junxian Pan Yongjian Ye +4 位作者 Mengzhen Zhou Xiang Sun Yihan Ling Keiji Yashiro Yan Chen 《Materials Reports(Energy)》 2021年第2期35-47,共13页
Solid oxide cells(SOCs)have attracted great attention in the past decades because of their high conversion efficiency,low environmental pollution and diversified fuel options.Nickel-based catalysts are the most widely... Solid oxide cells(SOCs)have attracted great attention in the past decades because of their high conversion efficiency,low environmental pollution and diversified fuel options.Nickel-based catalysts are the most widely used fuel electrode materials for SOCs due to the low price and high activity.However,when hydrocarbon fuels are employed,nickel-based electrodes face serious carbon deposition challenges,leading to a rapid decline of cell performance.Great efforts have been devoted to understanding the occurrence of the coking reaction,and to improving the stability of the electrodes in hydrocarbon fuels.In this review,we summarize recent research progress of utilizing surface modification to improve the stability and activity of Ni-based electrodes for SOCs by preventing carbon coking.The review starts with a briefly introduction about the reaction mechanism of carbon deposition,followed by listing several surface modification technologies and their working principles.Then we introduce representative works using surface modification strategies to prevent carbon coking on Ni-based electrodes.Finally,we highlight future direction of improving electrode catalytic activity and anti-coking performance through surface engineering. 展开更多
关键词 Solid oxide cells Ni-based electrodes Carbon coking surface engineering
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Nano-surface Engineering for Remanufacturing Application
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作者 ZHANG Wei(张伟) +3 位作者 XU Bin-shi(徐滨士) ZHANG Shu(张纾) 《Journal of Shanghai Jiaotong university(Science)》 EI 2005年第4期397-401,共5页
As system of a serial of technologies and engineering activities, remanufacturing aims at restoring and rebuilding waste machinery through advanced technologies and industrialized measures under the direction of the p... As system of a serial of technologies and engineering activities, remanufacturing aims at restoring and rebuilding waste machinery through advanced technologies and industrialized measures under the direction of the product total life cycle theory. With the development of surface engineering, nano-surface engineering has been one subject of intensive studies. In addition, nano-surface engineering has become an important means for property reforming and promoting of remanufacturing parts. Many low-dimension and nano-size or nano-structure functional coatings, which can improve materials properties evidently, are deposited by new methods. In this paper, some researches about the new achievement and remanufacturing application of the nano-stmctured coatings by different nano-surface engineering technologies in our laboratory were introduced. Especially, nano-structured DLC multilayer coatings by d.c. plasma CVD, nano-composed Al2O3/Ni, SiC/Ni and Diamond/Ni coatings by brush plating, and nano-composed Al2O3/TiO2 coating by plasma spraying were introduced in detail. 展开更多
关键词 REMANUFACTURING surface engineering chemical vapour deposition (CVD) brush plating plasma spraying
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Surface Molecular Encapsulation with Cyclodextrin in Promoting the Activity and Stability of Fe Single-Atom Catalyst for Oxygen Reduction Reaction
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作者 Changli Chen Haijing Li +5 位作者 Jingzhao Chen Dong Li Wenxing Chen Juncai Dong Mengru Sun Yujing Li 《Energy & Environmental Materials》 SCIE EI CAS CSCD 2023年第2期303-310,共8页
Fe single-atom catalysts(Fe-SACs)have been extensively studied as a highly efficient electrocatalyst toward the oxygen reduction reaction(ORR).Nonetheless,they suffer from stability issue induced by dissolution of Fe ... Fe single-atom catalysts(Fe-SACs)have been extensively studied as a highly efficient electrocatalyst toward the oxygen reduction reaction(ORR).Nonetheless,they suffer from stability issue induced by dissolution of Fe metal center and the OH^(−)blocking.Herein,a surface molecular engineering strategy is developed by usingβ-cyclodextrins(CDs)as a localized molecular encapsulation.The CD-modified Fe-SAC(Fe-SNC-β-CD)shows obviously improved activity toward the ORR with 0.90 V,4.10 and 4.09 mA cm^(-2)for E_(1/2),J_(0)and Jk0.9,respectively.Meanwhile,the Fe-SNC-β-CD shows the excellent long-term stability against aggressive stress and the poisoning.It is confirmed through electrochemical investigation that modification ofβ-CD can,on one hand,regulate the atomic Fe coordination chemistry through the interaction between the CD and FeN_(x) moiety,while on the other mitigate the strong adsorption of OH^(−)and function as protective barrier against the poisoning molecules leading to enhanced ORR activity and stability for the Fe-SACs.The molecular encapsulation strategy demonstrates the uniqueness of post-pyrolysis surface molecular engineering for the design of single-atom catalyst. 展开更多
关键词 oxygen reduction reaction singe atom catalyst STABILITY surface molecular engineering
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Spontaneous hierarchical surface engineering of minerals through coupled dissolution-precipitation chemistry 被引量:1
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作者 Jinyang Jiang Jiawen Zhang +4 位作者 Lanxin Wang Zeyu Lu Fengjuan Wang Zhiyong Liu Hongbo Zeng 《Aggregate》 EI CAS 2024年第1期460-472,共13页
Peculiar hierarchical microstructures in creatures inspire modern material design with distinct functionalities.Creatures can effortlessly construct sophisticated yet long-range ordered microstructure across bio-membr... Peculiar hierarchical microstructures in creatures inspire modern material design with distinct functionalities.Creatures can effortlessly construct sophisticated yet long-range ordered microstructure across bio-membrane through ion secretion and precipitation.However,microstructure biomimicry in current technology generally requires elaborate,point-by-point fabrication.Herein,a spontaneous yet controllable strategy is developed to achieve surface microstructure engineering through a natural surface phenomenon similar to ion secretion-precipitation,that is,coupled dissolution-precipitation.A series of hierarchical microstructures on mineral surfaces in fluids with tunable morphology,orientation,dimension,and spatial distribution are achieved by simply controlling initial dissolution and fluid chemistry.In seawater,long-range ordered film of vertically aligned brucite flakes forms through interfacial dissolution,nucleation,and confinement-induced orientation of flakes with vertically grown{110}plane,on the edge of which,fusiform aragonite epitaxially precipitates.With negligible initial surface dissolution,prismatic aragonite epitaxially grows on a calcite polyhedron-packed surface.By tuning fluid chemistry,closely packed calcite polyhedron and loosely packed calcite micro-pillars are engineered through rapid and retarded precipitation,respectively.Surprisingly,the spontaneously grown microstructures resemble those deliberately created by human or found in nature,and tremendously modulate surface functionality.These findings open new possibilities for facile and customizable engineering of microstructural surfaces,hierarchical heterostructures,and biomimetic materials. 展开更多
关键词 directional crystallization dissolution-precipitation chemistry hierarchical microstructures spontaneous growth surface engineering
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Surface/Interface Engineering of Hierarchical MoO_(2)/MoNi_(4)@Ru/RuO_(2)Heterogeneous Nanosheet Arrays for Alkaline Water Electrolysis with Fast Kinetics 被引量:1
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作者 Qiong Zhang Ruixue Zhang +6 位作者 Yingxiu Zhao Tiantian Sun Jianyang Gao Guang-Rui Xu Zexing Wu Yu Yang Lei Wang 《Chinese Journal of Chemistry》 SCIE CAS CSCD 2024年第2期119-128,共10页
Realizing the hydrogen economy by water electrolysis is an attractive approach for hydrogen production,while the efficient and stable bifunctional catalysts under high current densities are the bottleneck that limits ... Realizing the hydrogen economy by water electrolysis is an attractive approach for hydrogen production,while the efficient and stable bifunctional catalysts under high current densities are the bottleneck that limits the half-cell reactions of water splitting.Here,we propose an approach of hydrothermal and thermal annealing methods for robust MoO_(2)/MoNi_(4)@Ru/RuO_(2) heterogeneous cuboid array electrocatalyst with multiplying surface-active sites by depositing a monolayer amount of Ru.Benefiting from abundant MoO_(2)/MoNi_(4)@Ru/RuO_(2)heterointerfaces,MoO_(2)/MoNi_(4)@Ru/RuO_(2) heterogeneous cuboid array electrocatalysts effectively drive the alkaline water splitting with superior hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)performances.The synthesized MoO_(2)/MoNi_(4)@Ru/RuO_(2) has high HER activity,which realizes the working overpotentials of 48 mV at 50 mA·cm^(-2),further achieving overpotentials of 230 mv for industry-level 1000 mA·cm^(-2) in alkaline water electrolysis.Moreover,it also showed an enhanced OER activity than commercial RuO_(2) with a small overpotential of 280 mV at 200 mA·cm^(-2) in alkaline media.When building an electrolyzer with electrodes of(-)MoO_(2)/MoNi_(4)@Ru/RuO_(2)IIMo02/MoNig@Ru/RuO_(2)(+),a cell voltage of 1.63 V and 1.75 V is just required to support the current density of 200 mA·cm^(-2) and 500 mA-cm^(-2) in alkaline water electrolysis,much lower than that of the electrolyzer of(-)Pt/CIIRuO_(2)(+).This work demonstrates that MoO_(2)/MoNig@Ru/RuO_(2) heterogeneous nanosheet arrays are promising candidates for industrial water electrolysis applications,providing a possibility for the exploration of water electrolysis with a large currentdensity. 展开更多
关键词 Hierarchical heterostructure surface engineering Bifunctional catalysts Hydrogen evolution reaction Oxygen evolution reaction Watersplitting Catalytic activity ELECTROCATALYSIS Heterogeneous catalysis
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Surface engineering with ionic polymers on membranes for boron removal
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作者 Xiting Zhang Chenyi Fang +1 位作者 J Paul Chen Sui Zhang 《Frontiers of Chemical Science and Engineering》 SCIE EI CSCD 2024年第5期61-69,共9页
Removal of boric acid from seawater and wastewater using reverse osmosis membrane technologies is imperative and yet remains inadequately addressed by current commercial membranes.Existing research efforts performed p... Removal of boric acid from seawater and wastewater using reverse osmosis membrane technologies is imperative and yet remains inadequately addressed by current commercial membranes.Existing research efforts performed post-modification of reverse osmosis membranes to enhance boron rejection,which is usually accompanied by substantial sacrifice in water permeability.This study delves into the surface engineering of low-pressure reverse osmosis membranes,aiming to elevate boron removal efficiency while maintaining optimal salt rejection and water permeability.Membranes were modified by the self-polymerization and co-deposition of dopamine and polystyrene sulfonate at varying ratios and concentrations.The surfaces became smoother and more hydrophilic after modification.The optimum membrane exhibited a water permeability of 9.2±0.1 L·m^(-2)·h^(-1)·bar^(-1),NaCl rejection of 95.8%±0.3%,and boron rejection of 49.7%±0.1% and 99.6%±0.3% at neutral and alkaline pH,respectively.The water permeability is reduced by less than 15%,while the boron rejection is 3.7 times higher compared to the blank membrane.This research provides a promising avenue for enhancing boron removal in reverse osmosis membranes and addressing water quality concerns in the desalination process. 展开更多
关键词 MEMBRANE low-pressure reverse osmosis BORON surface engineering
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Surface engineering on MnO_(2)nanorods by La single atoms to accelerate oxygen reduction kinetics
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作者 Zhang-Long He Liu-Qi Wang +10 位作者 Min Jiang Jia-Nan Xie Shan Liu Jin-Can Ren Rui Sun Wen-Bin Lv Wei-Bin Guo Yu-Ling Liu Bing Li Qi Liu Hao He 《Rare Metals》 SCIE EI CAS CSCD 2024年第9期4302-4311,共10页
Surface engineering,which modulates the electronic structure and adsorption/desorption properties of electrocatalysts,is one of the key strategies for improving the catalytic performance.Herein,we demonstrate a facile... Surface engineering,which modulates the electronic structure and adsorption/desorption properties of electrocatalysts,is one of the key strategies for improving the catalytic performance.Herein,we demonstrate a facile solid-phase reaction for surface engineering of MnO_(2)to boost the oxygen reduction kinetics.Via reaction with surface hydroxy groups,La single atoms with loading amount up to 2.7 wt%are anchored onto a-MnO_(2)nanorods.After surface engineering,the oxygen reduction reaction(ORR)kinetics is significantly improved with the half-wave potential from 0.70 to 0.84 V,the number of transferred electrons from 2.5 to 3.9 and the limiting current density from 4.8 to 6.0 mA·cm^(-2).In addition,the catalyst delivers superior discharge performance in both alkaline and neutral metal–air batteries.Density functional theory(DFT)calculations reveal that atomic La modulates the surface electronic configuration of MnO_(2),reduces its d-band center and thus lowers the OOH*and O*reaction energy barrier.This work provides a new route for rational design of highly active electrocatalyst and holds great potential for application in various catalytic reactions. 展开更多
关键词 surface engineering Single atoms Electron injection Oxygen reduction reaction Metal-air batteries
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Surface engineering of 1D nanocatalysts for value-added selective electrooxidation of organic chemicals
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作者 Yongping Yang Chuhao Liu +2 位作者 Tinglu Song Mufan Li Zipeng Zhao 《Nano Research》 SCIE EI CSCD 2024年第3期1327-1336,共10页
Electrolytic water splitting by renewable energy is a technology with great potential for producing hydrogen(H_(2))without carbon emission,but this technical route is hindered by its huge energy(electricity)cost,which... Electrolytic water splitting by renewable energy is a technology with great potential for producing hydrogen(H_(2))without carbon emission,but this technical route is hindered by its huge energy(electricity)cost,which is mainly wasted by the anode oxygen evolution reaction(OER)while the value of the anode product(oxygen)is very limited.Replacing the high-energy-cost OER with a selective organic compound electrooxidation carried out at a relatively lower potential can reduce the electricity cost while producing value-added chemicals.Currently,H_(2) generation coupled with synthesis of value-added organic compounds faces the challenge of low selectivity and slow generation rate of the anodic products.One-dimensional(1D)nanocatalysts with a unique morphology,well-defined active sites,and good electron conductivity have shown excellent performance in many electrocatalytic reactions.The rational design and regulation of 1D nanocatalysts through surface engineering can optimize the adsorption energy of intermediate molecules and improve the selectivity of organic electrooxidation reactions.Herein,we summarized the recent research progress of 1D nanocatalysts applied in different organic electrooxidation reactions and introduced several different fabrication strategies for surface engineering of 1D nanocatalysts.Then,we focused on the relationship between surface engineering and the selectivity of organic electrooxidation reaction products.Finally,future challenges and development prospects of 1D nanocatalysts in the coupled system consisting of organic electrooxidation and hydrogen evolution reactions are briefly outlined. 展开更多
关键词 hydrogen generation organic compound electrooxidation one-dimensional(1D)nanocatalysts surface engineering SELECTIVITY
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