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Key role of electron accessibility at the noble metal-free catalytic interface in hydrogen evolution reaction

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Nano Research 2024年第4期17卷 2538-2545页

作者： Dongchen Han Nanxing Gao Yuyi Chu Zhaoping Shi Ying Wang Junjie Ge Meiling Xiao Changpeng Liu Wei Xing State Key Laboratory of Electroanalytical Chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China School of applied Chemistry and engineering University of Science and Technology of ChinaHefei 230026China Laboratory of Advanced Power Sources Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China Jilin Province Key Laboratory of Low Carbon Chemical Power Sources Changchun 130022China State Key Laboratory of Rare Earth Resource Utilization Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China

The reactant concentration at the catalytic interface holds the key to the activity of electrocatalytic hydrogen evolution reaction(HER),mainly referring to the capacity of adsorbing hydrogen and electron *** hydrogen adsorption free energy(ΔGH)as a reactivity descriptor,the volcano curve based on Sabatier principle is established to evaluate the hydrogen evolution activity of ***,the role of electron as reactant received insufficient attention,especially for noble metal-free compound catalysts with poor conductivity,leading to cognitive gap between electronic conductivity and apparent catalytic *** we successfully construct a series of catalyst models with gradient conductivities by regulating molybdenum disulfide(MoS_(2))electronic bandgap via a simple solvothermal *** demonstrate that the conductivity of catalysts greatly affects the overall catalytic *** further elucidate the key role of intrinsic conductivity of catalyst towards water electrolysis,mainly concentrating on the electron transport from electrode to catalyst,the electron accumulation process at the catalyst layer,and the charge transfer progress from catalyst to *** and experimental evidence demonstrates that,with the enhancement in electron accessibility at the catalytic interface,the dominant parameter governing overall HER activity gradually converts from electron accessibility to combination of electron accessibility and hydrogen adsorbing *** results provide the insight from various perspective for developing noble metal-free catalysts in electrocatalysis beyond HER.

关键词： conductivity molybdenum disulfide catalytic interface electron accessibility hydrogen evolution charge transfer.

Unlocking the potential of ultra-thin two-dimensional antimony materials:Selective growth and carbon coating for efficient potassium-ion storage

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Journal of Energy Chemistry 2024年第5期92卷 440-449页

作者： Dongyu Zhang Zhaomin Wang Yabin Shen Yeguo Zou Chunli Wang Limin Wang Yong Cheng State Key Laboratory of Rare Earth Resource Utilization Changchun Institute of Applied ChemistryChinese Academy of Sciences(CAS)Changchun 130022JilinChina School of applied Chemistry and engineering University of Science and Technology of ChinaHefei 230026AnhuiChina

Antimony-based anodes have attracted wide attention in potassium-ion batteries due to their high theoretical specific capacities(∼660 mA h g^(-1))and suitable voltage ***,severe capacity fading caused by huge volume change and limited ion transportation hinders their practical ***,strategies for controlling the morphologies of Sb-based materials to improve the electrochemical performances have been *** these,the two-dimensional Sb(2D-Sb)materials present excellent properties due to shorted ion immigration paths and enhanced ion ***,the synthetic methods are usually tedious,and even the mechanism of these strategies remains elusive,especially how to obtain large-scale 2D-Sb ***,a novel strategy to synthesize 2D-Sb material using a straightforward solvothermal method without the requirement of a complex nanostructure design is *** method leverages the selective adsorption of aldehyde groups in furfural to induce crystal growth,while concurrently reducing and coating a nitrogen-doped carbon *** to the reported methods,it is simpler,more efficient,and conducive to the production of composite nanosheets with uniform thickness(3–4 nm).The 2D-Sb@NC nanosheet anode delivers an extremely high capacity of 504.5 mA h g^(-1) at current densities of 100 mA g^(-1) and remains stable for more than 200 *** characterizations and molecular dynamic simulations,how potassium storage kinetics between 2D Sb-based materials and bulk Sb-based materials are explored,and detailed explanations are *** findings offer novel insights into the development of durable 2D alloy-based anodes for next-generation potassium-ion batteries.

关键词： Antimony Two-dimensional materials Selective growth Nitrogen-doped carbon Potassium-ion batteries

Synergetic Control of Li+ Transport Ability and Solid Electrolyte Interphase by Boron-Rich Hexagonal Skeleton Structured All-Solid-State Polymer Electrolyte

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Energy & Environmental Materials 2024年第3期7卷 158-167页

作者： Yanan Li Shunchao Ma Yuehua Zhao Silin Chen Tingting Xiao Hongxing Yin Huiyu Song Xiumei Pan Lina Cong Haiming Xie Department of Chemistry National & Local United Engineering Laboratory for Power BatteryNortheast Normal University State Key Laboratory of Electroanalytical Chemistry Changchun Institute of Applied Chemistry Chinese Academy of Sciences

High Li+transference number electrolytes have long been understood to provide attractive candidates for realizing uniform deposition of Li+.However,such electrolytes with immobilized anions would result in incomplete solid electrolyte interphase （SEI） formation on the Li anode because it suffers from the absence of appropriate inorganic components entirely derived from anions ***,a boron-rich hexagonal polymer structured all-solid-state polymer electrolyte （BSPE+ 10%LiBOB）with regulated intermolecular interaction is proposed to trade off a high Li+transference number against stable SEI *** Li+transference number of the as-prepared electrolyte is increased from 0.23 to 0.83 owing to the boron-rich cross-linker （BC） *** intriguingly,for the first time,the experiments combined with theoretical calculation results reveal that BOB-anions have stronger interaction with B atoms in polymer chain than TFSI-,which significantly induce the TFSI-decomposition and consequently increase the amount of LiF and Li3N in the SEI ***,a LiFePO4|BSPE+ 10%LiBOBlLi cell retains 96.7%after 400 cycles while the cell without BC-resisted electrolyte only retains 40.8%.BSPE+ 10%LiBOB also facilitates stable electrochemical cycling of solid-state Li-S *** study blazes a new trail in controlling the Li+transport ability and SEI properties,synergistically.

关键词： all-solid-state electrolyte boron-rich polymer lithium metal batteries lithium-ion transference number solid electrolyte interphase layer

Catalytic activation of peroxodisulfate using shape-controlled cerium-manganese composite oxide for phenol degradation:Kinetics and degradation pathway investigation

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Journal of Rare Earths 2024年第8期42卷 1514-1523,I0004页

作者： Yanxia Zheng Lixi Yang Chuxin Huang Yuchao Li Cuncun Zuo Tingting Ge Haofei Huang Jiutao An Ming Wang Yansong Zhao institute of Clean Chemical Technology School of Chemistry and Chemical EngineeringShandong University of TechnologyZibo255000China Shandong Collegial engineering Research Center of Novel Rare Earth Catalysis Materials Shandong University of TechnologyZibo255000 China College of Resources and Environment engineering Shandong University of TechnologyZibo255000China Department of Safety Chemistry and Biomedical Laboratory SciencesFaculty of Engineering and ScienceWestern Norway University of Applied Sciences(HVL)5063BergenNorway

Phenol-containing wastewater is typical organic wastewater,and its treatment is *** advanced method to treat this type of wastewater is persulfate *** friendly ceriummanganese composite oxide materials were synthesized by hydrothermal method and applied to the phenol degradation *** ratios of cerium and manganese,as well as the amount of sodium hydroxide,were *** solid solutions of cerium and manganese were formed and confirmed by X-ray diffraction(XRD) and transmission electron microscopy(TEM).H_(2)-temperature programmed reduction(H_(2)-TPR) and X-ray photoelectron spectroscopy(XPS) were utilized to analyze the synergistic effect of cerium and *** is found that there is a transformation between Ce^(4+)/Ce^(3+) and Mn^(2+)/Mn^(3+),which makes the material more trivalent manganese and thereby increases the catalytic *** effect of materials in catalyzing phenol degradation by peroxodisulfate(PDS) under various preparation conditions is discussed and high-effciency removal of phenol can be achieved and the removal rate at 180 min is close to 100%.The kinetic of this process was investigated and activation energy of phenol degradation is 62,35 kJ/*** degradation pathway of phenol was studied and it is found that PDS can be activated by low metal ions and the OH and SO_(4·)^(-)radicals play crucial roles according to the quenching experiments.

关键词： Advanced oxidation process Persulfate Mn-Ce solid solution Phenol degradation Rare earths

Structural engineering of Anode Materials for Low-Temperature Lithium-Ion Batteries:Mechanisms,Strategies,and Prospects

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Nano-Micro Letters 2024年第8期16卷 169-195页

作者： Guan Wang Guixin Wang Linfeng Fei Lina Zhao Haitao Zhang Beijing Key Laboratory of Ionic Liquids Clean process Institute of Process EngineeringChinese Academy of SciencesBeijing 100190People’s Republic of China School of Chemical engineering Sichuan UniversityChengdu 610065People’s Republic of China School of Energy Materials and Chemical engineering Hefei UniversityHefei 230601People’s Republic of China School of Materials Science and engineering Nanchang UniversityNanchang 330031People’s Republic of China Key Laboratory of Polymer and Catalyst Synthesis Technology of Liaoning Province School of Environmental and Chemical EngineeringShenyang University of TechnologyShenyang 110870People’s Republic of China

The severe degradation of electrochemical performance for lithium-ion batteries(LIBs)at low temperatures poses a significant challenge to their practical ***,extensive efforts have been contributed to explore novel anode materials with high electronic conductivity and rapid Li^(+)diffusion kinetics for achieving favorable low-temperature performance of ***,we try to review the recent reports on the synthesis and characterizations of low-temperature anode ***,we summarize the underlying mechanisms responsible for the performance degradation of anode materials at subzero ***,detailed discussions concerning the key pathways(boosting electronic conductivity,enhancing Li^(+)diffusion kinetics,and inhibiting lithium dendrite)for improving the low-temperature performance of anode materials are ***,several commonly used low-temperature anode materials are briefly ***,recent progress in the engineering of these low-temperature anode materials is summarized in terms of structural design,morphology control,surface&interface modifications,and multiphase ***,the challenges that remain to be solved in the field of low-temperature anode materials are *** review was organized to offer valuable insights and guidance for next-generation LIBs with excellent low-temperature electrochemical performance.

关键词： Low-temperature performance Anode materials Microstructural regulations Surface modifications

High-efficiency crystalline white organic lightemitting diodes

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Light(Science & Applications) 2024年第4期13卷 747-759页

作者： Yijun Liu Feng Zhu Yue Wang Donghang Yan State Key Laboratory of Polymer Physics and Chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China. School of applied Chemistry and engineering University of Science and Technology of ChinaHefei 230026China. State Key Laboratory of Supramolecular Structure and Materials Jilin UniversityChangchun 130012China

Crystalline white organic light-emitting diodes(C-WOLEDs)are promising candidates for lighting and display *** is urgently necessary,however,to develop energy-saving and high-efficiency C-WOLEDs that have stable and powerful emission to meet commercial ***,we report a crystalline host matrix(CHM)with embedded nanoaggregates(NA)structure for developing high-performance C-WOLEDs by employing a thermally activated delayed fluorescence(TADF)material and orange phosphorescent dopants(Phos.-D).The CHM-TADFNA-D WOLED exhibit a remarkable EQE of 12.8%,which is the highest performance WOLEDs based on crystalline *** device has a quick formation of excitons and a well-designed energy transfer process,and possesses a fast ramping of luminance and current *** to recently reported high-performance WOLEDs based on amorphous material route,the C-WOLED achieves a low series-resistance Joule-heat loss ratio and an enhanced photon output,demonstrating its significant potential in developing the next-generation WOLEDs.

关键词： diodes dopant crystalline

Atomically dispersed Fe sites on hierarchically porous carbon nanoplates for oxygen reduction reaction

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Journal of Energy Chemistry 2024年第3期90卷 7-15,I0002页

作者： Ruixue Zheng Qinglei Meng Hao Zhang Teng Li Di Yang Li Zhang Xiaolong Jia Changpeng Liu Jianbing Zhu Xiaozheng Duan Meiling Xiao Wei Xing State Key Laboratory of Electroanalytical Chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022JilinChina School of applied Chemistry and engineering University of Science and Technology of ChinaHefei 230026AnhuiChina Laboratory of Advanced Power Sources Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022JilinChina institute of Functional Nano&Soft Materials(FUNSOM) Jiangsu Key Laboratory for Carbon-Based Functional Materials&DevicesJiangsu Key Laboratory of Advanced Negative Carbon TechnologiesSoochow UniversitySuzhou 215123JiangsuChina State Key Laboratory of Polymer Physics and Chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022JilinChina

Developing cost-effective,robust and stable non-precious metal catalysts for oxygen reduction reaction(ORR) is of paramount importance for electrochemical energy conversion devices such as fuel cells and metal-air *** Fe-N-C single atom catalysts(SACs) have been hailed as the most promising candidate due to the optimal binding strength of ORR intermediates on the Fe-N_(4) sites,they suffer from serious mass transport limitations as microporous templates/substrates,i.e.,zeolitic imidazolate frameworks(ZIFs),are usually employed to host the active *** by this challenge,we herein develop a hydrogen-bonded organic framework(HOF)-assisted pyrolysis strategy to construct hierarchical micro/mesoporous carbon nanoplates for the deposition of atomically dispersed Fe-N_(4) *** a design is accomplished by employing HOF nanoplates assembled from 2-aminoterephthalic acid(NH_(2)-BDC) and p-phenylenediamine(PDA) as both soft templates and C,N *** from the structural merits inherited from HOF templates,the optimized catalyst(denoted as Fe-N-C SAC-950) displays outstanding ORR activity with a high half-wave potential of 0.895 V(*** hydrogen electrode(RHE)) and a small overpotential of 356 mV at 10 mA cm^(-2) for the oxygen evolution reaction(OER).More excitingly,its application potential is further verified by delivering superb rechargeability and cycling stability with a nearly unfading charge-discharge gap of 0.72 V after 160 *** dynamics(MD) simulations reveal that micro/mesoporous structure is conducive to the rapid mass transfer of O_(2),thus enhancing the ORR *** situ Raman results further indicate that the conversion of O_(2) to~*O_(2)-the rate-determining step(RDS) for Fe-N-C *** work will provide a versatile strategy to construct single atom catalysts with desirable catalytic properties.

关键词： Fe single atom catalysts Oxygen reduction reaction Mesoporous structure Active sites Zinc-air battery

Heteroepitaxial growth of Au@Pd core–shell nanocrystals with intrinsic chiral surfaces for enantiomeric recognition

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Rare Metals 2024年第1期43卷 225-235页

作者： Feng-Xia Wu Feng-Hua Li Xia-Li Lv Qi-Xian Zhang Guo-Bao Xu Wen-Xin Niu State Key Laboratory of Electroanalytical Chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China Shaoxing institute of Technology Shanghai UniversityShaoxing 312000China university of Science and Technology of China Hefei 230026China School of Materials Science and engineering Shanghai UniversityShanghai 200436China Zhejiang institute of Advanced Materials Shanghai UniversityJiashan 314113China university of Chinese Academy of sciences Beijing 100039China

Noble metal surfaces with intrinsic chirality serve as an ideal candidate for investigating enantioselective chemistry due to their superior chemical durability and high catalytic ***,significant advance has been made in synthesizing metal nanocrystals with intrinsic ***,the majority reports are limited to ***,through a heteroepitaxial growth strategy,the synthesis of metal nanocrystals with intrinsic chirality to palladium was extended for the first time and their application in enantioselective recognition was *** heteroepitaxial growth strategy allows for transferring the chirality of homochiral Au nanocrystals to Au@Pd core–shell *** employing the chiral Au@Pd nanocrystals as enantiomeric recognizing elements,a series of electrochemical sensors for chiral discrimination were *** optimal conditions,the peak potential between D-dihydroxyphenylalanine(D-DOPA)and L-dihydroxyphenylalanine(L-DOPA)is about 80 m V,and the peak current of D-DOPA is 2 times as much as that of L-DOPA,which enables the determination of the enantiomeric excess(EE,%)of ***,this report not only introduces a heteroepitaxial growth strategy to synthesize metal nanocrystals with intrinsic chirality,but also demonstrates the superior capability of integrating intrinsic chirality and catalytic properties into metal nanocrystals for chiral recognition.

关键词： Core–shell nanostructures Chirality transfer electrochemical sensors Chiral recognition Chiroplasmonics

Exploring the impact of Nafion modifier on electrocatalytic CO_(2) reduction over Cu catalyst

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Journal of Energy Chemistry 2024年第1期88卷 543-551,I0012页

作者： Yingshi Su Yonghui Cheng Zhen Li Yanjia Cui Caili Yang Ziyi Zhong Yibing Song Gongwei Wang Lin Zhuang College of Chemistry&Chemical engineering and Key Laboratory for Preparation and Application of Ordered Structural Materials of Guangdong Province Shantou UniversityShantou 515063GuangdongChina College of Chemistry and Molecular sciences Hubei Key Lab of Electrochemical Power SourcesWuhan UniversityWuhan 430072HubeiChina The institute for Advanced Studies Wuhan UniversityWuhan 430072HubeiChina Department of Chemistry engineering Guangdong Technion-Israel Institute of Technology(GTIIT)Shantou 515063GuangdongChina Technion-Israel institute of Technology(IIT) Haifa 32000Israel

Nafion as a universal polymer ionomer was widely applied for nanocatalysts electrode ***,the effect of Nafion on electrocatalytic performance was often overlooked,especially for CO_(2)***,the key roles of Nafion for CO_(2)RR were systematically studied on Cu nanoparticles(NPs)*** found that Nafion modifier not only inhibit hydrogen evolution reaction(HER)by decreasing the accessibility of H_(2)O from electrolyte to Cu NPs,and increase the CO_(2)concentration at electrocatalyst interface for enhancing the CO_(2)mass transfer process,but also activate CO_(2)molecule by Lewis acid-base interaction between Nafion and CO_(2)to accelerate the formation of^(*)CO,which favor of C–C coupling for boosting C_(2)product *** to these features,the HER selectivity was suppressed from 40.6%to 16.8%on optimal Cu@Nafion electrode at-1.2 V versus reversible hydrogen electrode(RHE),and as high as 73.5%faradaic efficiencies(FEs)of C_(2)products were achieved at the same applied potential,which was 2.6 times higher than that on bare Cu electrode(~28.3%).In addition,Nafion also contributed to the long-term stability by hinder Cu NPs morphology ***,this work provides insights into the impact of Nafion on electrocatalytic CO_(2)RR performance.

关键词： Nafion modifier CO_(2)reduction Cu nanoparticles In situ ATR-SEIRAS C_(2)product