Interfacial synergy of ultralong jagged Pt85Mo15-S nanowires with abundant active sites on enhanced hydrogen evolution in an alkaline solution
Interfacial synergy of ultralong jagged Pt85Mo15-S nanowires with abundant active sites on enhanced hydrogen evolution in an alkaline solution
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具有丰富活性位点的超长锯齿状 Pt85Mo15-S 纳米线的界面协同作用增强碱性溶液中的析氢
DOI：
10.1039/c9ta09285d
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发表时间：
2019
影响因子：
11.9
通讯作者：
Li Jun
中科院分区：
文献类型：
--
作者：
Wang Yao;Zhuo Hongying;Zhang Xin;Li Yunrui;Yang Juntao;Liu Yujie;Dai Xiaoping;Li Mingxuan;Zhao Huihui;Cui Meilin;Wang Hai;Li Jun
pt基催化剂在碱性介质中较高的析氢电催化活性很大程度上取决于其内在的微观表面化学环境。考虑到Pt与亲氧组分之间界面相互作用的基本机理，设计一个适度的亲氧表面环境有利于Pt在析氢反应（HER）中具有较高的催化活性。本文以S为“活性助剂”，制备了具有丰富界面活性位点的超长锯齿状Pt85Mo15-S纳米线，以增强催化HER性能。引人注目的是，Pt85Mo15-S纳米线的活性是商用Pt/C的3.62倍比电流密度和4.03倍质量电流密度，并且具有优异的碱性HER稳定性。x射线光电子能谱显示，S元素可以阻止Mo进一步氧化，从而导致Mo向Pt转移足够的电子。此外，理论计算表明，在Pt与MoSx密切接触的界面协同作用下，水解离能垒可以显著降低。本工作为推进电催化材料基础研究开辟了新的思路，为碱性HER基础电催化研究提供了系统的界面模型催化剂构建方法。
The higher electrocatalytic activity of hydrogen evolution in basic media for Pt-based catalysts is largely dependent on the intrinsic microscopic surface chemical environment. Given the fundamental mechanism of the interfacial interaction between Pt and oxophilic components, engineering a moderate oxygen-friendly surface environment of Pt-based catalysts is beneficial for endowing Pt with high catalytic activity for the hydrogen evolution reaction (HER). Herein, we fabricated ultralong jagged Pt85Mo15–S nanowires with rich interfacial active sites by using S as the “active auxiliary” to demonstrate an enhanced catalytic HER performance. Strikingly, the Pt85Mo15–S nanowires exhibited exceptional activity with 3.62 times the specific current density and 4.03 times the mass current density of commercial Pt/C as well as excellent stability towards alkaline HER. X-ray photoelectron spectroscopy revealed that the S element could prevent the further oxidization of Mo and then lead to enough electron transfer from Mo to Pt. In addition, the theoretical calculations demonstrated that the water dissociation energy barrier could be significantly reduced under the interfacial synergy of the intimate contact between Pt and MoSx. This work illustrates a new strategy to advance the fundamental exploration on electrocatalytic materials, which makes a systematic approach to build an interfacial model catalyst for fundamental electrocatalytic studies of alkaline HER.