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Oxidation Evolution and Activity Origin of N-Doped Carbon in the Oxygen Reduction Reaction

Transactions of Tianjin University 2024年第4期30卷 369-379页

作者： Jiaqi Wu chuanqi cheng Shanshan Lu Bin Zhang Yanmei Shi Department of Chemistry School of ScienceInstitute of Molecular PlusTianjin UniversityTianjin 300072China School of Materials Science and Engineering Institute of New Energy MaterialsTianjin UniversityTianjin 300072China Tianjin Key Laboratory of Molecular Optoelectronic Science Collaborative Innovation Center of Chemical Science and EngineeringTianjin 300072China

N-doped carbon materials,with their applications as electrocatalysts for the oxygen reduction reaction(ORR),have been extensively ***,a negletcted fact is that the operating potential of the ORR is higher than the theoretical oxida-tion potential of carbon,possibly leading to the oxidation of carbon ***,the infl uence of the structural oxidation evolution on ORR performance and the real active sites are not *** this study,we discover a two-step oxida-tion process of N-doped carbon during the *** fi rst oxidation process is caused by the applied potential and bubbling oxygen during the ORR,leading to the oxidative dissolution of N and the formation of abundant oxygen-containing functional *** oxidation process also converts the reaction path from the four-electron(4e)ORR to the two-electron(2e)***,the enhanced 2e ORR generates oxidative H_(2)O_(2),which initiates the second stage of oxidation to some newly formed oxygen-containing functional groups,such as quinones to dicarboxyls,further diversifying the oxygen-containing functional groups and making carboxyl groups as the dominant *** also reveal the synergistic eff ect of multiple oxygen-containing functional groups by providing additional opportunities to access active sites with optimized adsorption of OOH*,thus leading to high effi ciency and durability in electrocatalytic H_(2)O_(2) production.

关键词： Oxygen reduction reaction N-doped carbon Reaction path Structural evolution Oxidation in reduction

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Engineering Ru(IV)charge density in Ru@RuO2 core-shell electrocatalyst via tensile strain for efficient oxygen evolution in acidic media

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Chinese Journal of Catalysis 2020年第8期41卷 1161-1167页

作者： Yizhi Wen Tao Yang chuanqi cheng Xueru Zhao Enzuo Liu Jing Yang Institute of New-Energy Materials Key Laboratory of Advanced Ceramics and Machining Technology of Ministry of EducationSchool of Materials Science and EngineeringTianjin UniversityTianjin 300072China

The design of efficient Ru-based electrocatalysts with high intrinsic activities for acidic water oxidation is highly desirable and challenging for water splitting in proton exchange membrane ***,for the first time,we engineer the charge density of Ru(IV)by creating tensile strains in the RuO2 shell of Ru@RuO2 core-shell nanoparticles,***@***-resolution spectroscopic characterizations confirm the presence of av.6%tensile strain in Ru-O bonds,which results in an effective reduction of the Ru(IV)charge *** resultant Ru^X+(4

关键词： Tensile strain Core-shell structure Ruthenium oxide Charge density Oxygen evolution reaction Acidic media

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Electrosynthesis of hydroxylamine from nitrate reduction in water

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Science China Chemistry 2023年第6期66卷 1758-1762页

作者： Xianen Lan chuanqi cheng chengying Guo Minghao Guo Tieliang Li Yongmeng Wu Yifu Yu Bin Zhang Institute of Molecular Plus Department of ChemistrySchool of ScienceTianjin UniversityTianjin 300072China Institute of New Energy Materials School of Materials Science and EngineeringTianjin UniversityTianjin 300072China Haihe Laboratory of Sustainable Chemical Transformations Tianjin 300192China

Hydroxylamine(NH_(2)OH),a vital but unstable industrial feedstock,is presently prepared under harsh conditions that cause environmental and energy ***,we report an electrochemical method to prepare oximes,which serve as precursors for NH_(2)OH after facile *** carbon-supported amorphous Mn electrocatalyst delivers a current density of~100 mA cm^(-2) with a Faradaic efficiency of 40.92%and a yield rate of 0.251 mmol cm^(-2)h^(-1) for formaldoxime(CH_(2)NOH)generation by using nitrate and formaldehyde as *** can be easily released to produce NH_(2)OH via ***,this method exhibits an economic advantage over conventional manufacturing based on techno-economic analysis.A series of control experiments,in situ characterizations,and theoretical simulations unveil the reaction mechanism via the spontaneous reaction between an aldehyde and*NH_(2)OH intermediate derived from nitrate *** high activity of Mn originates from its inhibitory effects on the further reduction of key*NH_(2)OH *** strategy opens a sustainable and green way for NH_(2)OH synthesis under mild conditions using renewable energy.

关键词： electrosynthesis hydroxylamine nitrate reduction amorphous Mn reaction pathway

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Hydrogen-assisted activation of N_(2)molecules on atomic steps of ZnSe nanorods

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Nano Research 2023年第5期16卷 6721-6727页

作者： Kun Du Xiuyao Lang Yuanyuan Yang chuanqi cheng Ning Lan Kangwen Qiu Jing Mao Weichao Wang Tao Ling Key Laboratory for Advanced Ceramics and Machining Technology of Ministry of Education Institute of New-EnergySchool of Materials Science and EngineeringTianjin UniversityTianjin 300072China Tianjin Key Laboratory of Photo-Electronic Thin Film Device and Technology College of Electronic Information and Optical Engineering Nankai UniversityTianjin 300071China College of Energy Engineering Huanghuai UniversityZhumadian 463000China

Electrochemical reduction reaction of nitrogen(NRR)offers a promising pathway to produce ammonia(NH_(3))from renewable ***,the development of such process has been hindered by the chemical inertness of N_(2).It is recently proposed that hydrogen species formed on the surface of electrocatalysts can greatly enhance ***,there is still a lack of atomiclevel connection between the hydrogenation behavior of electrocatalysts and their NRR ***,we report an atomistic understanding of the hydrogenation behavior of a highly twinned ZnSe(T-ZnSe)nanorod with a large density of surface atomic steps and the activation of N_(2)molecules adsorbed on its *** theoretical calculations and in situ infrared spectroscopic characterizations suggest that the atomic steps are essential for the hydrogenation of T-ZnSe,which greatly reduces its work function and efficiently activates adsorbed N_(2)***,the liquid-like and free water over T-ZnSe promotes its *** a result,T-ZnSe nanorods exhibit significantly enhanced Faradaic efficiency and NH3 production rate compared with the pristine ZnSe *** work paves a promising way for engineering electrocatalysts for green and sustainable NH3 production.

关键词： electrocatalytic nitrogen reduction reaction atomic steps work function ZnSe

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Dynamically modulated synthesis of hollow metal-organic frameworks for selective hydrogenation reactions

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Nano Research 2023年第8期16卷 11334-11341页

作者： Liyun Xiao chuanqi cheng Zhixi Li Chaoyang Zheng Jing Du Meina Song Yue Wan Shaopeng Li Guo Jun Meiting Zhao Department of Chemistry Institute of Molecular Aggregation ScienceTianjin Key Laboratory of Molecular Optoelectronic SciencesTianjin UniversityTianjin 300072China Institute of New Energy Materials School of Materials Science and EngineeringTianjin UniversityTianjin 300072China State Key Laboratory of Separation Membranes and Membrane Processes School of ChemistryTiangong UniversityTianjin 300387China

Hollow metal-organic frameworks(MOFs)have attracted increasing attention in the field of catalysis in recent years due to their unique cavity structure with fast mass-diffusion rates and easily accessible active ***,we report the use of dynamic modulators,which are formed by the in-situ imine condensation reaction of 4-aminobenzoic acid and 4-formylbenzoic acid,to regulate the growth of MOFs to synthesize well-defined hollow thioether functionalized UiO-67(denoted as H-UiO-67-S)single *** supporting Pd nanoparticles,the designed catalysts Pd@H-UiO-67-S show excellent conversion(>99.9%),selectivity(>99.9%),and stability(10 cycles)in the selective hydrogenation of nitrobenzenes with other reducible *** functional theory calculations and the experimental results reveal that Pd nanoparticles not only selectively adsorb the nitro-groups on nitrobenzene,but also restrict the adsorption of the aniline product,due to the interaction of thioether with Pd in the confined pores of H-UiO-67-S,finally result in a significant increase in selectivity of nitro-hydrogenation.

关键词： hollow structure metal-organic frameworks(MOFs) dynamically modulated synthesis selective hydrogenation nitrobenzene

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Dual-site collaboration boosts electrochemical nitrogen reduction on Ru-S-C single-atom catalyst

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Chinese Journal of Catalysis 2022年第12期43卷 3177-3186页

作者： Liujing Yang chuanqi cheng Xun Zhang cheng Tang Kun Du Yuanyuan Yang Shan-cheng Shen Shi-Long Xu Peng-Fei Yin Hai-Wei Liang Tao Ling Key Laboratory for Advanced Ceramics and Machining Technology of Ministry of Education Institute of New-EnergySchool of Materials Science and EngineeringTianjin UniversityTianjin 300072China School of Chemical Engineering and Advanced Materials The University of AdelaideAdelaideSA 5005Australia Department of Chemistry University of Science and Technology of ChinaHefei 230026AnhuiChina

Electrocatalytic reduction of nitrogen into ammonia(NH_(3))is a highly attractive but challenging route for NH_(3)*** propose to realize a synergetic work of multi reaction sites to overcome the limitation of sustainable NH_(3)***,using ruthenium-sulfur-carbon(Ru-S-C)catalyst as a prototype,we show that the Ru/S dual-site cooperates to catalyse eletrocatalytic nitrogen reduction reaction(eNRR)at ambient *** the combination of theoretical calculations,in situ Raman spectroscopy,and experimental observation,we demonstrate that such Ru/S dual-site cooperation greatly facilitates the activation and first protonation of N_(2)in the rate-determining step of *** a result,Ru-S-C catalyst exhibits significantly enhanced eNRR performance compared with the routine Ru-N-C catalyst via a single-site catalytic *** anticipate that our specifically designed dual-site collaborative catalytic mechanism will open up a new way to offers new opportunities for advancing sustainable NH_(3)production.

关键词： Ru/S dual-site mechanism Electronic‘push-push’mechanism Electrocatalytic nitrogen reduction reaction

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Simultaneously achieving high energy density and responsivity in submicron BaTiO_(3) film capacitors integrated on Si

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Journal of Advanced Ceramics 2024年第2期13卷 198-206页

作者： Jun Ouyang Yinxiu Xue chuanqi Song Meiling Yuan Kun Wang Yuyao Zhao Hongbo cheng Hanfei Zhu Chao Liu Institute of Advanced Energy Materials and Chemistry School of Chemistry and Chemical EngineeringQilu University of Technology(Shandong Academy of Sciences)Jinan 250353China Key Laboratory of Key Film Materials&Application for Equipment School of Material Sciences and EngineeringXiangtan UniversityXiangtan 411105China School of Materials Science and Engineering Shandong UniversityJinan 250061China Academic Affairs Office Civil Aviation University of ChinaTianjin 300300China China Tobacco Shandong Industrial Co. Ltd.Jinan 250014China

In the research field of energy storage dielectrics,the“responsivity”parameter,defined as the recyclable/recoverable energy density per unit electric field,has become critically important for a comprehensive evaluation of the energy storage capability of a *** this work,high recyclable energy density and responsivity,i.e.,W_(rec)=161.1 J·cm^(-3) and ξ=373.8 J·(kV·m^(2))^(-1),have been simultaneously achieved in a prototype perovskite dielectric,BaTiO_(3),which is integrated on Si at 500℃ in the form of a submicron thick *** ferroelectric film features a multi-scale polar structure consisting of ferroelectric grains with different orientations and inner-grain ferroelastic domains.A LaNiO_(3) buffer layer is used to induce a{001}textured,columnar nanograin microstructure,while an elevated deposition temperature promotes lateral growth of the nanograins(in-plane diameter increases from~10-20 nm at lower temperatures to~30 nm).These preferably oriented and periodically regulated nanograins have resulted in a small remnant polarization and a delayed polarization saturation in the film’s P-E behavior,leading to a high recyclable energy ***,an improved polarizability/dielectric constant of the BaTiO_(3) film has produced a much larger maximum polarization than those deposited at lower temperatures at the same electric field,leading to a record-breaking responsivity for this simple perovskite.

关键词： energy storage energy density responsivity BaTiO_(3) dielectric capacitor Si

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Dielectric ultracapacitors based on columnar nano-grained ferroelectric oxide films with gradient phases along the growth direction

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Journal of Advanced Ceramics 2024年第7期13卷 1072-1079页

作者： chuanqi Song Feifan Zheng Yuan Zhang Hongbo cheng Long Teng Kun Wang Hanfei Zhu Chao Liu Li Wang Zhengyan Liang Jun Ouyang Institute of Advanced Energy Materials and Chemistry School of Chemistry and Chemical EngineeringQilu University of Technology(Shandong Academy of Sciences)Jinan 250353China Department of Materials Science and Engineering Southern University of Science and TechnologyShenzhen 518055China Key Laboratory of Key Film Materials&Application for Equipment(Hunan Province) School of Materials Science and EngineeringXiangtan UniversityXiangtan 411105China China Tobacco Shandong Industrial Co. Ltd.Jinan 250104China

In this work,dielectric ultracapacitors were designed and fabricated using a combination of phase boundary and nanograin *** ultracapacitors are based on submicron-thick Ba(Zr_(0.2)Ti_(0.8))O_(3) ferroelectric films sputterdeposited on Si at 500℃.With a composition near a polymorphic phase boundary(PPB),a compressive strain,and a high nucleation rate due to the lowered deposition temperature,these films exhibit a columnar nanograined microstructure with gradient phases along the growth *** a microstructure presents three-dimensional polarization inhomogeneities on the nanoscale,thereby significantly delaying the saturation of the overall electric ***,a pseudolinear,ultraslim polarization(P)-electric field(E)hysteresis loop was obtained,featuring a high maximum applicable electric field(~5.7 MV/cm),low remnant polarization(~5.2μC/cm^(2))and high maximum polarization(~92.1μC/cm^(2)).This P-E loop corresponds to a high recyclable energy density(Wrec~208 J/cm^(3))and charge‒discharge efficiency(~88%).An indepth electron microscopy study revealed that the gradient ferroelectric phases consisted of tetragonal(T)and rhombohedral(R)polymorphs along the growth direction of the *** T-rich phase is abundant near the bottom of the film and gradually transforms into the R-rich phase near the *** films also exhibited a high Curie temperature of~460℃and stable capacitive energy storage up to 200℃.These results suggest a feasible pathway for the design and fabrication of high-performance dielectric film capacitors.

关键词： ferroelectric thin films energy storage phase coexistence nanograin silicon

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A Robust Gaussian Mixture Model for Mobile Robots’ Vision-based Pose Estimation

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Journal of Geodesy and Geoinformation Science 2019年第3期2卷 79-90页

作者： chuanqi cheng Xiangyang HAO Jiansheng LI Peng HU Xu ZHANG Engineering University of PAP Urumqi 830000 China Institute of Geographical Spatial Information Information Engineering University Zhengzhou 450001 China

In dynamic environments, the moving landmarks can make the accuracy of traditional vision-based pose estimation worse or even failure. To solve this problem, a robust Gaussian mixture model for vision-based pose estimation is proposed. The motion index is added to the traditional graph-based vision-based pose estimation model to describe landmarks’ moving probability, transforming the classic Gaussian model to Gaussian mixture model, which can reduce the influence of moving landmarks for optimization results. To improve the algorithm’s robustness to noise, the covariance inflation model is employed in residual equations. The expectation maximization method for solving the Gaussian mixture problem is derived in detail, transforming the problem into classic iterative least square problem. Experimental results demonstrate that in dynamic environments, the proposed method outperforms the traditional method both in absolute accuracy and relative accuracy, while maintains high accuracy in static environments. The proposed method can effectively reduce the influence of the moving landmarks in dynamic environments, which is more suitable for the autonomous localization of mobile robots.

关键词： vision-based navigation graph optimization pose estimation covariance inflation expectation maximization

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利用直线特征进行单幅图像畸变校正方法

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武汉大学学报（信息科学版） 2018年第1期43卷 60-66页

作者：赵漫丹张振杰程传奇郝向阳信息工程大学地理空间信息学院

针对传统镜头畸变校正方法较少,并考虑畸变中心带来的不利影响,提出了一种基于单幅图像直线特征的畸变校正方法,且能够同步地估计畸变系数和畸变中心。在单幅图像中建立单参数划分模型,深入分析了空间直线与畸变后直线的几何关系,证明... 详细信息

针对传统镜头畸变校正方法较少,并考虑畸变中心带来的不利影响,提出了一种基于单幅图像直线特征的畸变校正方法,且能够同步地估计畸变系数和畸变中心。在单幅图像中建立单参数划分模型,深入分析了空间直线与畸变后直线的几何关系,证明了空间三维直线经镜头畸变后,在二维平面形成圆弧,并且从该圆弧圆心为圆心的同心圆上的某点即是畸变中心,进而基于圆拟合方法对畸变参数进行估计。与已有方法相比,该方法考虑了畸变中心的影响,并且直接使用畸变点进行畸变参数估计,因此,具有更高的校正精度和更强的鲁棒性。实验中,首先对拟合图像进行实验,针对不同噪声、不同畸变系数对各种算法展开了三组仿真实验,结果表明,利用列文伯格马夸尔特（Levenberg-Marquardt,LM）算法进行圆拟合和畸变参数估计的方法性能表现良好。展开对真实黑白棋盘的畸变校正实验,运用三种算法对棋盘中13条直线进行畸变校正后的测量,表明LM算法要明显优于其他两种算法,有着良好的畸变校正效果。最后对真实场景的图片进行测试,取得了较为理想的畸变校正结果。

关键词：畸变校正径向畸变划分模型均方根误差

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