Stabilizing Highly Active Ru Sites by Suppressing Lattice Oxygen Participation in Acidic Water Oxidation
Stabilizing Highly Active Ru Sites by Suppressing Lattice Oxygen Participation in Acidic Water Oxidation
复制标题
通过抑制晶格氧参与酸性水氧化来稳定高活性 Ru 位点
DOI：
10.1021/jacs.1c00384
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发表时间：
2021
影响因子：
15
通讯作者：
Hu Yong F
中科院分区：
文献类型：
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作者：
Wen Yun Zhou;Chen Pei Ning;Wang Lu;Li Shang Yu;Wang Zi Yun;Abed Jehad;Mao Xin Nan;Min Yi Meng;Dinh Cao Thang;De Luna Phil;Huang Rui;Zhang Long Sheng;Wang Lie;Wang Li Ping;Nielsen Robert J.;Li Hui Hui;Zhuang Tao Tao;Ke Chang Chun;Voznyy Oleks;r;Hu Yong F
在制氢过程中，阳极析氧反应（OER）限制了质子交换膜水电解槽的能量转换效率，也影响了其稳定性。广泛使用的ir基催化剂存在活性不足的问题，而活性更高的ru基催化剂在OER条件下容易溶解。这与晶格氧的参与（晶格氧氧化机制（LOM））有关，这可能导致晶体结构崩溃，加速活性Ru物质的浸出，导致运行稳定性低。本研究开发的Sr-Ru-Ir三元氧化电催化剂在酸性电解液中具有较高的OER活性和稳定性。催化剂在10 mA cm - 2下的过电位达到190 mV，运行1500 h后过电位保持在225 mV以下。x射线吸收光谱和18o同位素标记在线质谱研究表明，晶格氧在OER过程中的参与被Ru-O-Ir局部结构中的相互作用所抑制，从而提供了稳定性如何提高的图片。Sr和Ir调节了活性Ru位点的电子结构，优化了OER含氧中间体的结合能。
In hydrogen production, the anodic oxygen evolution reaction (OER) limits the energy conversion efficiency and also impacts stability in proton-exchange membrane water electrolyzers. Widely used Ir-based catalysts suffer from insufficient activity, while more active Ru-based catalysts tend to dissolve under OER conditions. This has been associated with the participation of lattice oxygen (lattice oxygen oxidation mechanism (LOM)), which may lead to the collapse of the crystal structure and accelerate the leaching of active Ru species, leading to low operating stability. Here we develop Sr–Ru–Ir ternary oxide electrocatalysts that achieve high OER activity and stability in acidic electrolyte. The catalysts achieve an overpotential of 190 mV at 10 mA cm–2and the overpotential remains below 225 mV following 1,500 h of operation. X-ray absorption spectroscopy and18O isotope-labeled online mass spectroscopy studies reveal that the participation of lattice oxygen during OER was suppressed by interactions in the Ru–O–Ir local structure, offering a picture of how stability was improved. The electronic structure of active Ru sites was modulated by Sr and Ir, optimizing the binding energetics of OER oxo-intermediates.