Ultrahigh Pt-Mass-Activity Hydrogen Evolution Catalyst Electrodeposited from Bulk Pt
Ultrahigh Pt-Mass-Activity Hydrogen Evolution Catalyst Electrodeposited from Bulk Pt
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DOI：
10.1002/adfm.202112207
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发表时间：
2022-02-18
影响因子：
19
通讯作者：
Qin, Mingli
中科院分区：
文献类型：
--
作者：
Liu, Luan;Wang, Yan;Qin, Mingli
由于铂的稀缺性，最大化铂的利用率对于铂基析氢反应（HER）电催化剂的可规模实施至关重要。在这里，三个组件的异质结构HER催化剂与Pt-Pt质量活性，其中空心PtCu合金纳米球上的泡沫铜上的WO 3阵列上，进行了报道。已经指出，在先前的报道中，在评价催化剂在酸性介质中的HER性能中使用三电极配置中的Pt对电极具有污染工作电极的风险。在这里，作者合理地利用这种“污染”来“活化”低HER活性材料，最大化Pt利用率。其结果是，实现了Pt/C催化剂的质量活性，即在20和100 mV的过电位下分别为1.35和10.86 A mg（Pt）（-1），比商业Pt/C催化剂的质量活性高27和13倍，优于一些最先进的Pt-单原子催化剂。空心球结构和PtCu合金化增加了活性中心的数量和活性。密度泛函计算和电化学实验表明，WO 3和Pt之间的协同作用也是导致高HER活性的原因，其中氢溢出效应触发Volmer-Heyrovsky机制，促进H* 从Pt上快速去除，重新暴露活性位点。
Maximizing the Pt utilization is important for the widescale implementation of Pt-based hydrogen evolution reaction (HER) electrocatalysts, owing to the scarcity of Pt. Here, three-component heterostructured HER catalysts with ultrahigh Pt mass activity in which hollow PtCu alloy nanospheres are supported on an array of WO3 on Cu foam, are reported. It has been pointed out that the use of Pt counter electrode in a three-electrode configuration in evaluating catalysts' HER performances in acidic media carries the risk of contaminating the working electrode in previous reports. Here, the authors rationally utilize this "contaminating" to "activate" low-HER-activity materials, maximizing the Pt utilization. As a result, ultrahigh Pt mass activity is achieved, that is 1.35 and 10.86 A mg(Pt)(-1) at overpotentials of 20 and 100 mV, respectively, 27 and 13 times higher than those of commercial Pt/C catalysts, outperforming some state-of-the-art Pt-single-atom catalysts. The hollow sphere structure and PtCu alloying increase the number and reactivity of active sites. Density function calculations and electrochemical experiments reveal that the synergy between WO3 and Pt is also responsible for the high HER activity where the hydrogen spillover effect triggers the Volmer-Heyrovsky mechanism and promotes the rapid removal of H* from Pt to re-expose the active sites.