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Individually-atomic governing d-π*orbital interactions via Cupromoted optimization of Fe-d band centers for high-efficiency zinc-air battery

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Nano Research 2023年第4期16卷 4634-4642页

作者： Xinyan Zhou Kexin Song Yu Feng Chao Jiang zhongjun chen Zizhun Wang Nailin Yue Xin Ge Wei Zhang Weitao Zheng Key Laboratory of Automobile Materials MOE School of Materials Science&EngineeringJilin Provincial International Cooperation Key Laboratory of High-Efficiency Clean Energy MaterialsElectron Microscopy Centerand International Center of Future ScienceJilin UniversityChangchun 130012China Institute of High Energy Physics Chinese Academy of SciencesBeijing 100049China

It is challenging for precise governing of electronic configuration of the individually-atomic catalysts toward optimal electrocatalysis,as d-band configuration of a metal center determines the adsorption behavior of reactive species to the center in oxygen reduction reaction(ORR).The addition of Cu atom modifies the d-band center position of Fe central atom,thus strengthening the d-π*orbital ***,FeCu-NC catalyst in the nitrogen-doped carbon(NC)support containing individual dual-metal CuN4/FeN4 sites was prepared by the surface confinement strategy of zeolitic imidazolate framework(ZIF),treated as a model *** and theoretically co-verified dual-metal CuN4/FeN4 sites highly dispersed in the NC support,enable transferring more electrons from FeN4 sites to*OH intermediates,thereby accelerating the desorption process of*OH *** to those commercial Pt/C,Our FeCu-NC catalyst exhibited extraordinary ORR activity(with a E1/2 as high as 0.87 V)and cycling stability in 0.1 M KOH electrolyte,and thereof demonstrated excellent discharge performance in zinc-air *** construction of dual-atom catalysts(DACs)provides a strategy for atom-by-atom designing high-efficiency catalysts via orbital regulation.

关键词： dual-atom catalysts(DACs) electronic configuration oxygen reduction reaction(ORR) zinc-air battery

Copper-tetracyanoquinodimethane-derived copper electrocatalysts for highly selective carbon dioxide reduction to ethylene

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Nano Research 2022年第9期15卷 7910-7916页

作者： Xuewei Huang Dawei Wang Shuhao Yan Pengfei An Jianyu Han Zhiyu Guo Xinwei Li zhongjun chen Lin Chang Siyu Lu Zhiyong Tang Green Catalysis Center and College of ChemistryZhengzhou UniversityZhengzhou 450001China Henan Institute of Advanced Technology Zhengzhou UniversityZhengzhou 450001China CAS Key Laboratory of Nanosystem and Hierarchical Fabrication CAS Center for Excellence in NanoscienceNational Center for Nanoscience and TechnologyBeijing 100190China University of Chinese Academy of Sciences Beijing 100049China Institute of High Energy Physics Chinese Academy of Sciences Beijing 100049China

As one of the most promising CO_(2)utilization techniques,electrochemical CO_(2)reduction has recently received considerable *** is a unique electrocatalyst that can convert CO_(2)to value-added multi-carbon ***,Cu catalysts are always limited by the poor selectivity and ***,we report that using copper-tetracyanoquinodimethane(CuTCNQ)derived Cu nanoparticles as efficient electrocatalysts for conversion of CO_(2)to ethylene characteristic with high selectivity and stability,showing 56%Faradaic efficiency(FE)to C2H4 at−1.3 V *** hydrogen electrode(RHE).Upon the electrochemical CO_(2)reduction,CuTCNQ slowly reconstructs to Cu nanoparticles with abundant grain boundaries and residual Cu+on the *** calculation and operando characterization disclose that both as-formed Cu nanoparticle grain boundaries and residual Cu+endow the catalyst with high selectivity toward ***,during the reconstruction of CuTCNQ to Cu nanoparticles,the grain boundaries Cu surface is slowly refreshed by continual addition of Cu atoms,thus inhibiting the surface passivation and guaranteeing the electrocatalytic stability.

关键词： reconstruction grain boundary ethylene CO_(2)electroreduction

Study on the Treatment of Benign Prostate Hyperplasia Combined with Underactive Bladder Detrusor Contraction by Transurethral Plasma Enucleation of the Prostate

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Journal of Biosciences and Medicines 2023年第9期11卷 141-149页

作者： Yong Li zhongjun chen Department of Urology People’s Hospital of Songzi Jingzhou China

Objective: Exploring the clinical efficacy of transurethral plasma enucleation of the prostate in the treatment of benign prostatic hyperplasia with underactive bladder detrusor contractility. Methods: Retrospective analysis of the clinical data of 68 patients with benign prostatic hyperplasia and underactive detrusor muscle contractility treated by our department from July 2021 to July 2022. The above patients all met the diagnosis of benign prostatic hyperplasia, excluding prostate cancer and urethral stricture. Urodynamics showed a decrease in the contractile force of the bladder detrusor muscle, and the surgical equipment used Olympus bipolar plasma resection equipment method. Divide the above patients into two groups: the experimental group of 34 patients who underwent transurethral plasma enucleation of the prostate and the control group of 34 patients who underwent transurethral plasma resection of the prostate. Evaluate the preoperative clinical baseline level and postoperative observation indicators of the two groups of patients, and compare the statistical differences between the two groups. Results: Both groups of patients successfully completed the surgery, and there were no serious complications such as rectal or bladder perforation during the surgery, with less bleeding. The postoperative QOL, IPSS, Qmax, and residual urine volume of patients undergoing transurethral plasma enucleation and resection of the prostate were significantly improved compared to those before surgery (P 0.05). Conclusion: Transurethral enucleation of the prostate has good efficacy and safety in the treatment of benign prostatic hyperplasia combined with weakened detrusor muscle contractility. Compared with traditional electric resection surgery, the efficacy is more significant. In terms of the main complications of the surgery, although there are slightly more patients with temporary urinary incontinence after prostate enucleation, there is no statistically significant differe

关键词： Transurethral Enucleation of the Prostate Prostate Hyperplasia Underactive Bladder Detrusor Contractility

A novel SAXS/XRD/XAFS combined technique for in-situ timeresolved simultaneous measurements

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Nano Research 2023年第1期16卷 1123-1131页

作者： Zhonghua Wu Yunpeng Liu Xueqing Xing Lei Yao zhongjun chen Guang Mo Lirong Zheng Quan Cai Hao Wang Jiajun Zhong Yuecheng Lai Lixiong Qian Beijing Synchrotron Radiation Facility Institute of High Energy PhysicsChinese Academy of SciencesBeijing 100049China University of Chinese Academy of Sciences Chinese Academy of SciencesBeijing 100049China

Synchrotron radiation based combined technique can provide multiple structural information simultaneously,which is an important development direction of structural *** this study,a novel small-angle X-ray scattering/X-ray diffraction/X-ray absorption fine structure(SAXS/XRD/XAFS)combined setup was constructed,where an area detector,a curved detector,and a point detector are,respectively,used for the measurements of SAXS,XRD,and XAFS signals.A detailed description about the combined setup was given.A minitype diamond detector coupled to a SAXS beamstop was used to record the transmitted X-ray intensity,making the scattering(SAXS and XRD)signal measurement compatible with the absorption(XAFS)signal measurement,avoiding mechanical *** two-way sampling strategy was used to acquire XAFS signals,shortening the non-counting *** two-way and one-way sampling strategies were ***-frequency sampling scheme was used to collect experimental signals,improving the measurement efficiency and signal-to-noise ratio.A detailed description and discussion about the high-frequency scheme were also given in this *** the rotation of monochromator,there is no mechanical movement in measurements,time resolution may reach the level of *** this SAXS/XRD/XAFS combined setup,SAXS,XRD,and XAFS signals can be acquired *** some in-situ sample environment system,the newlydeveloped combined technique can be used to track the structure evolution in complex *** the formation processes of(BiO)2CO3 and ZnAPO-34 particles,the changes of in-situ experimental data with reaction time demonstrate that SAXS/XRD/XAFS combined technique is feasible to track the dynamic process.

关键词： SAXS/XRD/XAFS combined technique in-situ time-resolution

Optimizing high-coordination shell of Co-based single-atom catalysts for efficient ORR and zinc-air batteries

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Journal of Energy Chemistry 2024年第8期95卷 306-314,I0007页

作者： Yugang Qi Qing Liang Kexin Song Xinyan Zhou Meiqi Liu Wenwen Li Fuxi Liu Zhou Jiang Xu Zou zhongjun chen Wei Zhang Weitao Zheng Key Laboratory of Automobile Materials MOE School of Materials Science&Engineering Electron Microscopy Centerand International Center of Future ScienceJilin Provincial International Cooperation Key Laboratory of High-Efficiency Clean Energy MaterialsJilin UniversityChangchun 130012JilinChina Institute of High Energy Physics Chinese Academy of SciencesBeijing 100049China

Atom-level modulation of the coordination environment for single-atom catalysts(SACs)is considered as an effective strategy for elevating the catalytic *** the MNxsite,breaking the symmetrical geometry and charge distribution by introducing relatively weak electronegative atoms into the first/second shell is an efficient way,but it remains challenging for elucidating the underlying mechanism of ***,a practical strategy was reported to rationally design single cobalt atoms coordinated with both phosphorus and nitrogen atoms in a hierarchically porous carbon derived from metal-organic frameworks.X-ray absorption spectrum reveals that atomically dispersed Co sites are coordinated with four N atoms in the first shell and varying numbers of P atoms in the second shell(denoted as Co-N/P-C).The prepared catalyst exhibits excellent oxygen reduction reaction(ORR)activity as well as zinc-air battery *** introduction of P atoms in the Co-SACs weakens the interaction between Co and N,significantly promoting the adsorption process of ^(*)OOH,resulting in the acceleration of reaction kinetics and reduction of thermodynamic barrier,responsible for the increased intrinsic *** discovery provides insights into an ultimate design of single-atom catalysts with adjustable electrocatalytic activities for efficient electrochemical energy conversion.

关键词： Electrocatalytic Oxygen reduction reaction Single atom catalyst Shell coordination optimization

Efficient ORR catalysts for zinc-air battery: Biomass-derived ultra-stable Co nanoparticles wrapped with graphitic layers via optimizing electron transfer

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Journal of Energy Chemistry 2022年第7期31卷 211-218,I0006页

作者： Yu Feng Kexin Song Wei Zhang Xinyan Zhou Seung Jo Yoo Jin-Gyu Kim Sifan Qiao Yugang Qi Xu Zou zhongjun chen Tingting Qin Nailin Yue Zizhun Wang Dabing Li Weitao Zheng State Key Laboratory of Automotive Simulation and Control School of Materials Science&EngineeringKey Laboratory of Automobile Materials MOEElectron Microscopy Centerand International Center of Future ScienceJilin UniversityJilin UniversityChangchun 130012JilinChina Division of Scientific Instrumentation&Management Korea Basic Science InstituteDaejeon 34133Republic of Korea Institute of High Energy Physics Chinese Academy of SciencesBeijing 100049China State Key Laboratory of Luminescence and Applications Changchun Institute of OpticsFine Mechanics and PhysicsChinese Academy of SciencesChangchun 130033JilinChina

The poor stability of non-noble metal catalysts in oxygen reduction reaction(ORR) is a main bottleneck that limits their big-scale application in metal-air batteries. Herein, we construct a chainmail catalyst(Co-NC-AD) with outstanding stability, via the competitive complexation and post absorption strategy,consisting of highly graphitic layers wrapped uniform-size Co nanoparticles(Co-NPs). Experiments combined with density functional theory(DFT) calculations jointly confirmed that the electron transfer occurred from the inner Co-NPs to the external graphitic layers. It facilitated the adsorption process of oxygen molecules and the hybridization of the O-2 p and C-1 p orbitals, which accelerated the ORR reaction kinetics. Consequently, our prepared Co-NC-AD shows excellent ORR activity, offered with a more positive initial potential(E_(onset)= 0.95 V) and half-wave potential(E_(1/2)= 0.86 V). The remarkable stability and resistance of methanol poisoning are merited from the protection effect of stable graphitic layers. In addition, the high electrochemical performance of Co-NC-AD-based zinc-air battery demonstrates their potential for practical applications. Therefore, our work provides new ideas for the design of nanoconfined catalysts with high stability and activity.

关键词： Chainmail catalyst Graphitic layers Co nanoparticles Oxygen reduction reaction

Small-angle X-ray scattering study on the orientation of suspended sodium titanate nanofiber induced by applied electric field

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Radiation Detection Technology and Methods 2019年第3期3卷 148-154页

作者： Jiayi Wang Xiaoyi Zhao Yunpeng Liu Lixiong Qian Lei Yao Xueqing Xing Guang Mo Quan Cai zhongjun chen Zhonghua Wu Institute of High Energy Physics Chinese Academy of SciencesBeijing 100049China University of Chinese Academy of Sciences Beijing 100049China

Introduction Nanofiber orientation in suspensions determines the performance of nanoparticle suspensions which have potential applications in intelligent *** and method Na2Ti3O7 nanofibers were prepared with a hydrothermal *** orientation degree of Na2Ti3O7 nanofibers in silicone oil has been studied by in situ small-angle X-ray scattering ***ünemann–Ruland method was used to extract the distribution widths of Na2Ti3O7 nanofibers in the *** An empirical formula has been proposed to describe the dependence of nanofiber orientation degree on the external electric-field strength(E)and the nanofiber concentration(C).The results demonstrate that the response of nanofiber orientation to the electric field can be divided into exponential and linear stages before and after the inflection point of electric-field strength(Ec0.09 kV/mm).Low concentration of suspension is more sensitive to the external electric *** increase in nanofiber concentration will decrease the response sensitivity of nanofiber orientation degree to the change of *** critical concentration of Na2Ti3O7 nanofibers in the suspension is about 5 wt%.This study is expected to give new clue for the structurally responsive mechanism of anisotropic nanoparticles in suspensions to electric-field strength and particle concentration.

关键词： Orientation degree Suspension Nanofiber SAXS

Tuning the Surface Field by Embedding Cations into Metals to Direct the Reaction Pathway of CO_(2) Electroreduction

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CCS Chemistry 2024年第3期6卷 631-640页

作者： Pei Zhang Meng Zhou Shiqiang Liu Xueqing Xing Jiahao Yang Peng chen Yaoyu Yin Yingying cheng Xing Tong Jun Ma Qinggong Zhu Xiaofu Sun zhongjun chen Xinchen Kang Buxing Han Beijing National Laboratory for Molecular Sciences CAS Laboratory of Colloid and Interface and ThermodynamicsCAS Research/Education Center for Excellence in Molecular SciencesCenter for Carbon Neutral ChemistryInstitute of ChemistryChinese Academy of SciencesBeijing 100190 Beijing Synchrotron Radiation Facility Institute of High Energy PhysicsChinese Academy of SciencesBeijing 100049 Shanghai Key Laboratory of Green Chemistry and Chemical Processes School of Chemistry and Molecular EngineeringEast China Normal UniversityShanghai 200062 School of Chemistry University of Chinese Academy of SciencesBeijing 100049

The creation of universal strategies to affect the reaction route of the electroreduction of CO_(2) is ***,we report the first work to introduce cations into diverse metals such as Cu,Bi,In,and Sn via the electroreduction of related metallic oxides in quaternary ammonium surfactant *** to their physical adsorption,cations embedded into the electrodes have a more pronounced impact on the electrical field,which effectively influences the adsorption state of *** the increase of surface field,the hydrogen evolution reaction and*COOH route are significantly reduced,favouring the*OCHO pathway *** a result,hydrogen,CO,and C_(2+)products almost completely vanish at−0.5 V versus RHE in 0.1 M Na_(2)SO_(4)in an H-type cell after enough cations are embedded into the Cu electrode,and the faradaic efficiency of formate rises from 18.0%to 99.5%simultaneously.

关键词： CO_(2)electroreduction tuneable products electrical field reaction pathway cations embedding

Evaluation of the best follow-up period and curative effect for acoustic neuroma treated with a gamma knife

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The Chinese-German Journal of Clinical Oncology 2008年第9期7卷 515-518页

作者： Xi Li Yinhui Deng zhongjun Hou Yaotang chen Yong He Xiaojun Yu Gamma Knife Treatment and Research Center The Second Affiliated Hospital of Guangzhou Medical College Guangzhou 510260 China

Objective: To determine the best follow-up period with regard to curative effect for acoustic neuroma treated with a gamma knife. Methods: Sixty cases of acoustic neuroma were treated with a gamma knife. The follow-up period was from 3 to 102 months. Changes in the lesions and peripheral tissues and clinical symptoms were compared and the curative effectiveness of gamma knife treatment was evaluated. Results: The highest total effective rate (92.3%) was in the third period. There was a significant difference in the tumor size postoperatively. There was no edema in the peripheral tissues surrounding the tumor. It was not obvious that clinical symptoms changed. Conclusion: In this report, the best follow-up period was 24-36 months. Gamma knife treatment was still effective after 60 months post-operation.

关键词： acoustic neuroma gamma knife the best follow-up period