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Microenvironment regulation of M-N-C single-atom catalysts towards oxygen reduction reaction

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Nano Research 2023年第4期16卷 4468-4487页

作者： Li Zhang qinglei meng Ruixue Zheng Liuqing Wang Wei Xing Weiwei Cai Meiling Xiao State Key Laboratory of Electroanalytical Chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China Sustainable Energy Laboratory Faculty of Materials Science and ChemistryChina University of GeosciencesWuhan 430074China School of Applied Chemistry and Engineering University of Science and Technology of ChinaHefei 230026China

The development of cost-effective,robust,and durable electrocatalysts to replace the expensive Pt-based catalysts towards oxygen reduction reaction(ORR)is the trending frontier research topic in renewable energy and *** attention has been paid to metal-nitrogen-carbon(M-N-C)single atom catalysts(SACs)due to their maximized atom utilization efficiency,biomimetic active site,and distinct electronic *** importantly,their catalytic properties can be further tailored by rationally regulating the microenvironment of active sites(i.e.,M-N coordination number,heteroatom doping and ***,we present a comprehensive summary of the recent advancement in the microenvironment regulation of MN-C SACs towards improved ORR *** coordination environment manipulation regarding central metal and coordinated atoms is first discussed,focusing on the structure-function *** from the near-range coordination,longrange substrate modulation including heteroatom doping,defect engineering is discussed as ***,the synergy mechanism of nanoparticles and single atom sites to tune the electron cloud density at the active sites is ***,we provide the challenges and outlook of the development of M-N-C SACs.

关键词： single-atom catalyst oxygen reduction reaction microenvironment regulation active site structure electronic structure

A new pathway for formic acid electro-oxidation:The electro-chemically decomposed hydrogen as a reaction intermediate

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Journal of Energy Chemistry 2022年第8期31卷 188-191,I0006页

作者： Xiaolong Yang qinglei meng Xian Wang Zhao Jin Changpeng Liu Junjie Ge Wei Xing State Key Laboratory of Electroanalytical Chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022 Jilin China School of Applied Chemistry and Engineering University of Science and Technology of China

Formic acid electro-oxidation reaction(FAOR)is generally believed that follows a two-pathway ***,we resorted to in situ electrochemical mass spectrometry and successfully captured the trace of H_(2),as the new intermediate species,during the process of FAOR on both Pt based catalyst and two single atom catalysts(Rh-N-C and Ir-N-C).Inspired by this,we proposed a new reaction path named hydrogen oxidation pathway:at the oxidation potential,formic acid will break the C–H bond and combine with the protons in the solution to form H_(2) species,then hydrogen oxidation reaction(HOR)will occur to generate two *** process is accompanied by electron transfer and contributes currently to the whole reaction.

关键词： Formic acid electro-oxidation reaction Hydrogen Pt Single atom catalysts Reaction pathway

Revealing the true origin of size-dependent Pd/C catalytic behavior towards formic acid decomposition

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Chinese Chemical Letters 2023年第1期34卷 457-460页

作者： qinglei meng Xian Wang Meiling Xiao Zhao Jin Junjie Ge Changpeng Liu Wei Xing Laboratory of Advanced Power Sources Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China University of Science and Technology of China Hefei 230026China Jilin Province Key Laboratory of Low Carbon Chemical Power Sources Changchun 130022China State Key Laboratory of Electroanalytical Chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China

Formic acid decomposition(FAD)is considered a promising hydrogen production route to facilitate the ambient storage and on demand release of hydrogen *** optimize the catalysts for FAD,efforts have been paid to explore the underlying reason for the varied catalytic activity among catalysts with similar composition but differed ***,such endeavors are highly challenging due to the deeply intermingled effects of electronic structure,particle size,and facets,***,to separately evaluate the respective effects of these factors,a series of catalysts with the same surface electronic structure and different particle size was prepared by cation dipole adjustment *** performance and characterization results showed that the catalysts with different sizes and facets exhibited similar intrinsic activity with deviation of less than 5%.However,they showed 252%deviation of site stability,indicating that only the optimized electronic structure could enhance the intrinsic activity and a smaller particle size could extend the catalyst’s life.

关键词： Hydrogen production Formic acid Catalyst deactivation Size effect Facets effect

Fe,Cu-codoped metal-nitrogen-carbon catalysts with high selectivity and stability for the oxygen reduction reaction

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Chinese Chemical Letters 2021年第1期32卷 506-510页

作者： Yuemin Wang Ergui Luo Xian Wang qinglei meng Junjie Ge Changpeng Liu Wei Xing Laboratory of Advanced Power Sources Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China University of Science and Technology of China Hefei 230026China Jilin Province Key Laboratory of Low Carbon Chemical Power Sources Changchun 130022China State Key Laboratory of Electroanalytical Chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China

Metal-nitrogen-carbon materials(M-N-C) are non-noble-metal-based alternatives to platinum-based catalysts and have attracted tremendous attention due to their low-cost,high abundance,and efficient catalytic performance towards the oxygen reduction reaction(ORR).Among them,Fe-based materials show remarkable ORR activity,but they are limited by low selectivity and low *** address these issues,herein,we have synthesized FeCu-based M-N-C catalysts,inspired by the bimetal center of cytochrome c oxidase(CcO).In acidic media,the selectivity was notably improved compared with Febased materials,with peroxide yields less than 1.2%(<1/3 of the hydrogen peroxide yields of Fe-N-C catalysts).In addition to Cu-N-C catalysts which can catalytically reduce hydrogen peroxide,the reduction current of hydrogen peroxide using FeCu-N-C-20 exceeded that of Fe-N-C by about 6% when the potential was greater than 0.4 ***,FeCu-based M-N-C catalysts suffered from only a15 mV attenuation in their half-wave potentials after 10,000 cycles of accelerated degradation tests(ADT),while there was a 30 mV negative shift for ***,we propose that the H_(2)O_(2) released from Fe-Nx sites or N-doped carbon sites would be reduced by adjacent Cu-Nx sites,re sulting in low H_(2)O_(2) yields and high stability.

关键词： Fuel cell Oxygen reduction reaction Fe Cu-codoped metal-nitrogen-carbon catalysts High selectivity High stability

High-Performance Magnetic-core Coils for Targeted Rodent Brain Stimulations

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Biomedical Engineering Frontiers 2022年第1期3卷 82-92页

作者： Hedyeh Bagherzadeh qinglei meng Hanbing Lu Elliott Hong Yihong Yang Fow-Sen Choa Department of Computer Science and Electrical Engineering University of MarylandBaltimore CountyBaltimoreMD 21250USA Neuroimaging Research Branch National Institute on Drug AbuseNational Institutes of HealthBaltimoreMD 21224USA Maryland Psychiatric Research Center Department of PsychiatryUniversity of Maryland School of MedicineBaltimoreMD 21201USA

Objective and Impact *** is a need to develop rodent coils capable of targeted brain stimulation for treating neuropsychiatric disorders and understanding brain *** describe a novel rodent coil design to improve the focality for targeted stimulations in small rodent *** magnetic stimulation(TMS)is becoming increasingly important for treating neuropsychiatric disorders and understanding brain *** studies permit invasive manipulations and are essential for the mechanistic understanding of TMS effects and explorations of therapeutic outcomes in disease ***,existing TMS tools lack focality for targeted ***,there has been limited fundamental research on developing coils capable of focal stimulation at deep brain regions on small animals like *** this study,ferromagnetic cores are added to a novel angle-tuned coil design to enhance the coil performance regarding penetration depth and *** simulations and experimental electric field measurements were conducted to optimize the coil *** proposed coil system demonstrated a significantly smaller stimulation spot size and enhanced electric field decay rate in comparison to existing *** the ferromagnetic core reduces the energy requirements up to 60%for rodent brain *** simulated results are validated with experimental measurements and demonstration of suprathreshold rodent limb excitation through targeted motor cortex *** newly developed coils are suitable tools for focal stimulations of the rodent brain due to their smaller stimulation spot size and improved electric field decay rate.

关键词： stimulation manipulation becoming

Oxygen-vacancy-rich TiO_(2)enables highly active and durable water electrolysis of urchin-like RuO_(2)catalyst

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Science China(Technological Sciences) 2022年第10期65卷 2317-2324页

作者： GAO HongMei XIAO MeiLing LI GuoQiang GAO LiQin meng qinglei LUO ZhaoYan LUO ErGui LIU ChangPeng JIN Zhao GE JunJie XING Wei State Key Laboratory of Electroanalytical Chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China Laboratory of Advanced Power Sources Jilin Province Key Laboratory of Low Carbon Chemical Power SourcesChangchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China.

The material innovation is prerequisite to accelerating sluggish oxygen evolution reaction(OER)kinetics,thus promoting the realization of hydrogen energy ***,we develop an oxygen-vacancy-rich TiO_(2)supported RuO_(2)catalyst(RuO_(2)@r-TiO_(2))towards improved OER activity and *** oxygen vacancy on TiO_(2)not only supplies electrons to produce lower valence Ru,but also provides sufficient anchoring site for the deposition of RuO_(2)*** that,it can generate strong electronic interaction between TiO_(2)and supported RuO_(2),and thereby tailors the intermediates’adsorption energy on the RuO_(2)*** a result,the derived RuO_(2)@r-TiO_(2)catalyst exhibits superior OER activity and stability with the overpotential of 211 mV at a current density of 10 mA cm^(−2)and negligible activity degradation after 6 h operation,outperforming the non-oxygen-vacancy counterpart(223.3 mV,12.75%activity loss)and RuO_(2)catalyst(234.6 mV,42.86%activity loss).

关键词： oxygen evolution reaction oxygen vacancy electronic interaction stability

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

Full-length transcriptome sequencing analysis reveals differential skin color regulation in snakeheads fish Channa argus

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Aquaculture and Fisheries 2024年第4期9卷 590-596页

作者： Leigang Mao Yongan Zhu Jiaren Yan Longgang Zhang Shuren Zhu Li An qinglei meng Zhishan Zhang Xirong Wang College of Fisheries and Life Science Shanghai Ocean UniversityShanghai201306China Shandong Freshwater Fisheries Research Institute Jinan250017China

Albinism is a genetic disorder caused by a series of genetic abnormalities that result in a decrease in *** yellow snakehead fish(GCAS)has been discovered while the Channa argus(CAS)breeding,but the genetic mechanism that causes its albinism is not *** sequencing and comparison of CAS and GCAS skin using Oxford Nanopore Technologies(ONT)technology to elucidate the molecular mechanisms of snakehead albinism.27.1 G clean reads and 26,198 full-length non-redundant sequences were generated via ONT ***,8079 new transcripts and 7231 genes were identified by comparing and analyzing redundant removed transcripts and known reference genome *** results of DEGs analysis showed that a total of 59 transcripts were differentially expressed in the two groups,including 22 up-regulated transcripts and 37 down-regulated *** causative genes associated with albinism have been identified,including TYR(Tyrosinase)and SOX10(SRY-box transcription factor 10)(tyrosinase synthesis and metabolism),S-100(S100 calcium binding protein A1)(melanin production),NLRC3(NLR family CARD domain containing 3)(disease immunity)are significantly down-regulated in GCAS,while RhoGEFs expression(melanin synthesis)is *** interaction analysis revealed that GAPDH(Glyceraldehyde-3-phosphate dehydrogenase)is the top hub gene in the regulation of skin color in *** addition,the skin of snakehead fish is regulated by metabolic(GAPDH),immune[Tumor protein p53(TP53),C-X-C motif chemokine ligand 8(CXCL8),SRC proto-oncogene,non-receptor tyrosine kinase(SRC),CD274]and neural[Notch receptor 1(NOTCH1),C-X-C motif chemokine ligand 12(CXCL12)]related genes to achieve differences in skin *** findings in understanding the process by which albinism in fish develops.

关键词： Albinism Channa argus Nanopore-based RNA sequencing Melanin

Efficient Security Multimedia System on Embedded Platform

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China Communications 2010年第4期7卷 120-125页

作者： WANG Lifeng meng qinglei XIAO Chen MA Jian DU Yaogang WANG Wendong Beijing Electronic Science and Technology Institute Beijing 100070 China Institute of Network Technology Beijing University of Posts and Telecommunications Beijing 100876 China 706 Institute Second Academy of CASIC Beijing 100854 China School of Computer Science and Technology Bei Hang University Beijing 100083 China

Security video communication is a challenging task,especially for wireless video *** efficient security multimedia system on embedded platform is *** analyzing the hardware architecture and resource,the efficient DSP-based H.264/AVC coding is studied by efficient video coding techniques and system optimizing *** protect the confidentiality and integrity of media information,a novel security mechanism is presented,which includes user identify authentication and a perceptual video encryption algorithm based on exploiting the special feature of entropy coding in *** results show that the proposed hardware framework has high performance and achieves a better balance between security and *** proposed security mechanism can achieve high security and low complexity cost,and has a little effect on the compression ratio and transmission ***’s more,encoding and encryption at the same time,the performance of data process can meet real-time application.

关键词： H.264/AVC Encode Optimizing Encryption Identify Authentication