Boron-Induced Electronic-Structure Reformation of CoP Nanoparticles Drives Enhanced pH-Universal Hydrogen Evolution.,Angewandte Chemie International Edition

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Boron-Induced Electronic-Structure Reformation of CoP Nanoparticles Drives Enhanced pH-Universal Hydrogen Evolution.
Angewandte Chemie International Edition ( IF 16.1 ) Pub Date : 2019-12-21 , DOI: 10.1002/anie.201915254
Erping Cao ₁ , Zhimin Chen ₁ , Hao Wu ₁ , Peng Yu _{1,

2} , Ying Wang ₁ , Fei Xiao ₁ , Shuo Chen ₁ , Shichao Du ₁ , Ying Xie ₁ , Yiqun Wu ₁ , Zhiyu Ren ₁

Affiliation

Even though transition-metal phosphides (TMPs) have been developed as promising alternatives to Pt catalyst for the hydrogen evolution reaction (HER), further improvement of their performance requires fine regulation of the TMP sites related to their specific electronic structure. Herein, for the first time, boron (B)-modulated electrocatalytic characteristics in CoP anchored on the carbon nanotubes (B-CoP/CNT) with impressive HER activities over a wide pH range are reported. The HER performance surpasses commercial Pt/C in both neutral and alkaline media at large current density (>100 mA cm-2 ). A combined experimental and theoretical study identified that the B dopant could reform the local electronic configuration and atomic arrangement of bonded Co and adjacent P atoms, enhance the electrons' delocalization capacity of Co atoms for high electrical conductivity, and optimize the free energy of H adsorption and H2 desorption on the active sites for better HER kinetics.

中文翻译：

硼诱导的CoP纳米粒子的电子结构重整驱动了增强的pH值通用氢释放。

尽管已经开发出过渡金属磷化物（TMP）作为氢生成反应（HER）的Pt催化剂的有前途的替代品，但其性能的进一步提高仍需要对其特定电子结构相关的TMP位进行精细调节。在此，首次报道了锚固在碳纳米管（B-CoP / CNT）上的CoP中的硼（B）调节的电催化特性，在宽的pH范围内具有令人印象深刻的HER活性。在大电流密度（> 100 mA cm-2）下，在中性和碱性介质中，HER性能都超过了商用Pt / C。结合实验和理论研究表明，B掺杂剂可以改变键合Co和相邻P原子的局部电子构型和原子排列，增强电子的能级。

更新日期：2020-01-24

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