Modulating the Electrocatalytic Performance of Palladium with the Electronic Metal-Support Interaction: A Case Study on Oxygen Evolution Reaction
Modulating the Electrocatalytic Performance of Palladium with the Electronic Metal-Support Interaction: A Case Study on Oxygen Evolution Reaction
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通过电子金属-载体相互作用调节钯的电催化性能：析氧反应案例研究
DOI：
10.1021/acscatal.8b00460
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发表时间：
2018-07-01
期刊：
影响因子：
12.9
通讯作者：
Lv, Xiaojun
中科院分区：
文献类型：
--
作者：
He, Hongyang;Chen, Junxiang;Lv, Xiaojun
本文报道了一种通过引入金属-载体电子相互作用（EMSI）来调节贵金属的电子状态以提高其电催化性能的一般方法。作为一个案例研究，金属Pd对析氧反应（OER）在碱性溶液中的催化活性已显着提高稳定Pd δ +氧化物物种在Pd-金属氧化物载体的界面上的EMSI效应的帮助下，这表明在驱动OER的Pd δ +的内在优势。我们进一步证明，Pd δ +的化学状态可以很容易地调制在2+至3+的范围内，通过改变金属氧化物的支持，有趣的是，伴随着一个明确的依赖性的OER活性的Pd δ +的氧化态。高Pd ~（3+）含量的Fe_2O_3/Pd催化剂具有显著提高的OER性能，在10 mA cm ~（2）下显示出383 mV的过电位，相比之下，金属Pd上的过电位>600 mV，Fe_2O_3/玻碳上的过电位为540 mV。OER性能的极大提高被认为主要源于氧化中间体（例如，*OH和 *OOH）。此外，在碱性溶液中，在分别具有Au 3+、Pt 2+和Pt 4+的氧化物物种的Fe 2 O3/Au和Fe 2 O3/Pt上也实现了类似的EMSI诱导的OER活性的提高。
The present work reports a general approach to improve the electrocatalytic property of noble metal through regulating its electron status by introducing the electronic metalsupport interaction (EMSI). As a case study, the catalytic activity of metallic Pd toward oxygen evolution reaction (OER) in alkaline solution has been significantly promoted by stabilizing Pd delta+ oxidic species at the interface of the Pd-metal oxide support with the help of EMSI effect, suggesting an intrinsic advantage of Pd delta+ in driving OER. We further demonstrate that the chemical state of Pd delta+ can be easily modulated in the range of 2+ to 3+ by changing the metal oxide support, interestingly, accompanied by a clear dependence of the OER activity on the oxidation state of Pd delta+. The high Pd3+ species-containing Fe2O3/Pd catalyst has fed an impressively enhanced OER property, showing an overpotential of 383 mV at 10 mA cm(2) compared to those of >600 mV on metallic Pd and 540 mV on Fe2O3/glassy carbon. The greatly enhanced OER performance is believed to primarily derive from the distinctive improvement in the adsorption of oxygenated intermediates (e.g., *OH and *OOH) on metal-oxide/Pd catalysts. Moreover, similar EMSI induced improvements in OER activity in alkaline solution are also achieved on both of the Fe2O3/Au and Fe2O3/Pt, which possess the oxidic species of Au3+, and Pt2+ and Pt4+, respectively.