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Electrochemically Modifying the Electronic Structure of IrO_2 Nanoparticles for Overall Electrochemical Water Splitting with Extensive Adaptability

机译:电化学改性IRO_2纳米粒子的电子结构,具有广泛的适应性的整体电化学水分裂

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摘要

Designing the electrocatalysts that are stable and active for extensively adaptable water splitting is highly desirable for developing hydrogen based energy. IrO(2)is a promising and widely used catalyst for the oxygen evolution reaction in commercial applications, but is rarely used for the hydrogen evolution reaction (HER), due to the high Gibbs free energy for hydrogen adsorption (Delta G(H*)). Herein, an approach to modify the electronic structure of IrO(2)via cyclic voltammetry is proposed. In this process, Ir(+4) is partially reduced and trace Pt is simultaneously deposited on IrO2, which greatly lowers the Delta G(H*)and thus accelerates the reaction kinetics. The as-prepared Pt-IrO2/CC with low noble metal loading (36.6 mu g cm((Ir+Pt))(-2)) exhibits excellent HER activity with overpotentials of 5, 22, and 26 mV at 10 mA cm(-2)in 0.5mH(2)SO(4), 1mKOH, and 1mphosphate buffer solution, respectively, making it possible to organize an all-IrO(2)based water electrolyzer. The Pt-IrO2/CC||IrO2/CC couple exhibits a promising activity and stability in pH-universal conditions as well as natural seawater for H(2)production. Density function theory calculations reveal that the optimized electronic structure of IrO(2)balances the Delta G(H*), resulting in a much enhanced HER performance.
机译:设计稳定和活性为广泛适应性水分裂的电催化剂对于显影氢基能量非常希望。 IRO(2)是商业应用中的氧气进化反应的有前途和广泛使用的催化剂,但由于氢吸附的高吉布斯自由能量,很少用于氢进化反应(她)(ΔG(H *) )。这里,提出了一种通过循环伏安法修改IRO(2)的电子结构的方法。在该过程中,IR(+4)被部分地减少,并且在IRO 2上同时沉积痕量PT,这极大地降低了ΔG(H *),从而加速了反应动力学。具有低贵金属载荷(36.6μgcm((IR + Pt))( - 2))的AS制备的Pt-IrO2 / Cc表现出优异的她的活性,其过电位为5,22和26mV,10 mA cm( -2)分别在0.5mH(2)如此(4),1MKOH和1磷酸三磷酸盐缓冲溶液中,使得可以组织基于All-Iro(2)的水电解槽。 PT-IRO2 / CC || IRO2 / CC夫妇在pH-普通条件下表现出有希望的活性和稳定性,以及H(2)生产的天然海水。密度函数理论计算表明,IRO(2)的优化电子结构平衡了DELTA G(H *),从而提高了她的性能。

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  • 来源
    《Advanced energy materials》 |2020年第30期|2001600.1-2001600.9|共9页
  • 作者单位

    Xi An Jiao Tong Univ Sch Sci State Key Lab Mech Behav Mat Key Lab Shanxi Adv Mat & Mesoscop Phys Xian 710049 Peoples R China;

    Xi An Jiao Tong Univ Sch Sci State Key Lab Mech Behav Mat Key Lab Shanxi Adv Mat & Mesoscop Phys Xian 710049 Peoples R China;

    Xi An Jiao Tong Univ Sch Sci State Key Lab Mech Behav Mat Key Lab Shanxi Adv Mat & Mesoscop Phys Xian 710049 Peoples R China;

    Thermo Fisher Sci Bldg 8 399 Shengxia Rd Zhangjiang Hitech Pk Shanghai 201210 Peoples R China;

    Xi An Jiao Tong Univ Sch Sci State Key Lab Mech Behav Mat Key Lab Shanxi Adv Mat & Mesoscop Phys Xian 710049 Peoples R China;

    Xi An Jiao Tong Univ Sch Sci State Key Lab Mech Behav Mat Key Lab Shanxi Adv Mat & Mesoscop Phys Xian 710049 Peoples R China;

    Xi An Jiao Tong Univ Sch Sci State Key Lab Mech Behav Mat Key Lab Shanxi Adv Mat & Mesoscop Phys Xian 710049 Peoples R China|Xi An Jiao Tong Univ Shaanxi Quantong Joint Res Inst New Energy Vehicl Xian 710049 Peoples R China;

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  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类
  • 关键词

    DFT calculations; extensive adaptability; IrO2-based; overall water splitting;

    机译:DFT计算;广泛的适应性;基于IRO2;总水分裂;

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