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1能源电化学基础

界面电催化反应涉及界面电子转移(离子穿过双电层形成表面中间体)、化学反应(界面吸附物种相互反应)等多步过程,电极界面反应机制的研究可帮助了解电池能源充放电过程中电催化、吸附、溶解等涉及能源储存与转化的细节机理问题,通过原子级原位表面和光谱技术对电极反应过程中界面结构和化学中间物质的动力学过程追踪,揭示电极界面的反应机制。

 截屏2023-04-05 17.03.57.png  


(2) 贵金属电化学溶解

针对硫代硫酸盐浸金反应过程中界面硫钝化带来的生产过程的不稳定和钝化膜存在的溶金 反应动力学与机理不明确等问题,从冶金物理化学研究入手,通过原位追踪无氧环境中硫代硫 酸盐浸金界面溶金结构形貌的介观演化规律,探寻硫钝化界面溶金方式从溶金速率较慢的点蚀 向快速层状溶金演化的最佳条件。在对多长度尺度下浸金晶面硫 溶解及其结构演化、孔蚀到层状溶解演化的实验研究基础上,利用量子化学计算结合反应-输 运方程解析,从微观原子水平的物种吸附结构和电荷转移,到介观动态行为,再到宏观时空动力学进行模拟和理论分析,实现界面溶金机理阐明与定向调控。

Au(111)晶面电化学溶解的界面演化追踪

 截屏2023-04-05 17.04.10.png

a) 硫脲溶液中Au(111)晶面层状溶解向波状溶解的转变;b) 硫代硫酸盐浸金溶液中Au(111)晶面周期性孔蚀导致的层溶解


 

代表性论文:                           

 

(1)Sun xiao; Cao Xiru; Han Jiaxing; Ji Chen; Varela Hamilton; Del Colle Vinicius; Zhang Jiujun; Pan, Changwei*; Gao Qingyu*. Effect of Electrolyte Ions on Crystalline/Amorphous α-PtO2 Formation in the Electrocatalytic Oxidation of Pt(100) Preferentially Oriented NanoparticlesACS Catalysis 2023, 13, 14753-14762.

  (2) You, Xinyu; Han Jiaxing; Del Colle Vinicius; Xu Yuqiang; Chang Yanan; Sun Xiao; Wang Guichang; Ji Chen; Pan, Changwei*; Zhang, Jiujun*; Gao, Qingyu*. Relationship between oxide identity and electrocatalytic activity of platinum for ethanol electrooxidation in perchlorate acidic solution. Communication Chemistry 2023, 6, 101.

  (3) You, Xinyu; Xu Yuqiang, Han Jiaxing, Chang Yanan, Del Colle Vinicius; Ji Chen; Pan Changwei*; Zhang, Jiujun*; Gao, Qingyu*. Effect of Adsorbed Sulfate on the Product Selectivity of Ethanol Oxidation on Pt Nanoparticles in Acidic Solution. The Journal of Physical Chemistry C, 2023, 127(12): 5743-5753.https://pubs.acs.org/doi/10.1021/acs.jpcc.2c08881 

(4) You, Xinyu; Niu, Mingshuang; Del Colle, Vinicius; Sun, Xiao; Han, Jiaxzing; Ji, Chen; Pan, Changwei*; Zhang, Jiujun*; Gao, Qingyu*.Enhancement Effect of Chemisorbed Sulfate toward Electrochemical Oxidation of Ethanol on Platinum Electrodes. The Journal of Physical Chemistry C, 2022, 126(7): 3397-3403. https://pubs.acs.org/doi/10.1021/acs.jpcc.1c09960 

(5)Pan, Changwei; Niu, Mingshuang; Cui, Ruijun; Li, Lianqun; You, Xinyu; Sun, Xiao; Ji, Chen; Epstein, Irving R.; Gao, Qingyu*. Mesoscopic Pitting Oscillation-Induced Periodic Anodic Layer Electrodissolution of Au(111). The Journal of Physical Chemistry Letters, 2021, 12(50): 12062-12066.https://pubs.acs.org/doi/10.1021/acs.jpclett.1c03300 

(6) Li, Lianqun†; Pan, Changwei†; Shan, Jinju; She, Weibing; You, Xinyu; Ji, Chen; Gao, Qingyu.Pit-Induced Electrochemical Layer Dissolution and Wave Propagation on an Au(111) Surface in an Acidic Thiourea Solution. Journal of Physical Chemistry C, 2020, 124(35): 19112-19118.https://pubs.acs.org/doi/10.1021/acs.jpcc.0c05329 

(7) Ren, Lin; Wang, Liyuan; Gao, Qingyu; Teng, Rui; Xu, Ziyang; Wang, Jing; Pan, Changwei; Epstein, Irving R. Programmed Locomotion of an Active Gel Driven by Spiral Waves. Angewandte Chemie International Edition, 2020.

(8)Pan, Changwei; Lv, Fengpeng; Kegl, Tamas; Horvath, Attila K; Gao, Qingyu. Kinetics and Mechanism of the Concurrent Reactions of Hexathionate with S(IV) and Thiosulfate in a Slightly Acidic Medium. Journal of Physical Chemistry A, 2019, 123(26): 5418-5427.

(9)Zhang, Wei; Liu, Yang; Luo, Hainan; Pan, Changwei*. Effect of mass transfer process on hydrogen adsorption on polycrystalline platinum electrode in sulfuric acid solution. Chinese Chemical Letters, 2019, 30(6): 1168-1172.

(10)Cseko, Gyorgy; Pan, Changwei; Gao, Qingyu; Horvath, Attila K. Kinetics of the Two-Stage Oxidation of Sulfide by Chlorine Dioxide.Inorganic Chemistry, 2018, 57(16): 10189-10198.

(11)Liu, Yang; Yuan, Ling; Pan, Changwei; Gao, Jianmin; Zhou, Wenxiu; Gao, Qingyu. Photoinduced Oscillations and Pulse Waves in the Hydrogen Peroxide-Sulfite-Ferrocyanide Reaction.Journal of Physical Chemistry A, 2018, 122(5): 1175-1184. 

(12) Zhang, Wei; Pan, Changwei*; Gao, Qingyu. Chemisorbed Oxygen-Species-Mediated Electrocatalytic Oxidation of Thiourea and Thiosulfate. Journal of Physical Chemistry C, 2018, 122(42): 24150-24157. 

(13)Ren, Lin; Wang, Meng; Pan, Changwei; Gao, Qingyu; Liu, Yang; Epstein, Irving R. Autonomous reciprocating migration of an active material. Proceedings of the National Academy of Sciences of the United States of America, 2017, 114(33): 8704-8709. 

(14) Pan, Changwei; Cheng, Ruolan; Birzu, Adrian; Yang, Jiaping; Ren, Lin; Varela, Hamilton; Gao, Qingyu. Periodic Transition between Breathing Spots and Synchronous Sulfur Deposition/Dissolution in Transpassive Region of the Electro-Oxidation of Sulfide on Platinum. ChemElectroChem, 2017, 4(8): 2075-2078.