Li Huan, Hu Minghao, Cao Bo, Jing Peng, Liu Baocang, Gao Rui, Zhang Jun, Shi Xiaomeng, Du Yaping
School of Chemistry and Chemical Engineering & Inner Mongolia Engineering and Technology Research Center for Catalytic Conversion and Utilization of Carbon Resource Molecules, Inner Mongolia University, Hohhot, 010021, China.
Tianjin Key Lab for Rare Earth Materials and Applications, Center for Rare Earth and Inorganic Functional Materials, School of Materials Science and Engineering, National Institute for Advanced Materials, Nankai University, Tianjin, 300350, China.
Small. 2021 Mar;17(11):e2006617. doi: 10.1002/smll.202006617. Epub 2021 Feb 19.
A robust polyaniline-assisted strategy is developed to construct a self-supported electrode constituting a nitrogen, phosphorus, sulfur tri-doped thin graphitic carbon layer encapsulated sulfur-doped molybdenum phosphide nanosheet array (NPSCL@S-MoP NSs/CC) with accessible nanopores, desirable chemical compositions, and stable composite structure for efficient hydrogen evolution reaction (HER). The multiple electronic coupling effects of S-MoP with N, P, S tri-dopants afford effective regulation on their electrocatalytic performance by endowing abundant accessible active sites, outstanding charge-transfer property, and d-band center downshift with a thermodynamically favorable hydrogen adsorption free energy (ΔG ) for efficient hydrogen evolution catalysis. As a result, the NPSCL@S-MoP NSs/CC electrode exhibits overpotentials as low as 65, 114, and 49 mV at a geometric current density of 10 mA cm and small Tafel slopes of 49.5, 69.3, and 53.8 mV dec in 0.5 m H SO , 1.0 m PBS, and 1.0 m KOH, respectively, which could maintain 50 h of stable performance, almost outperforming all MoP-based catalysts reported so far. This study provides a valuable methodology to produce interacted multi-heteroatomic doped graphitic carbon-transition metal phosphide electrocatalysts with superior HER performance in a wide pH range.
开发了一种稳健的聚苯胺辅助策略，以构建一种自支撑电极，该电极由氮、磷、硫三掺杂的薄石墨碳层包裹硫掺杂的磷化钼纳米片阵列（NPSCL@S-MoP NSs/CC）组成，具有可及的纳米孔、理想的化学成分和稳定的复合结构，用于高效析氢反应（HER）。S-MoP与N、P、S三掺杂剂的多重电子耦合效应通过赋予丰富的可及活性位点、出色的电荷转移性能以及d带中心下移，从而具有热力学上有利的氢吸附自由能（ΔG），对其电催化性能进行有效调控，以实现高效析氢催化。结果，NPSCL@S-MoP NSs/CC电极在0.5 M H₂SO₄、1.0 M PBS和1.0 M KOH中，在几何电流密度为10 mA cm⁻²时，过电位分别低至65、114和49 mV，塔菲尔斜率分别为49.5、69.3和53.8 mV dec⁻¹，可保持50 h的稳定性能，几乎优于迄今为止报道的所有基于MoP的催化剂。本研究提供了一种有价值的方法来制备在宽pH范围内具有优异HER性能的相互作用的多杂原子掺杂石墨碳-过渡金属磷化物电催化剂。
