Pt single atoms meet metal-organic frameworks to enhance electrocatalytic hydrogen evolution activity

Jingting Zhu; Yingqian Cen; Haibin Ma; Weiguang Lian; Jidong Liu; Haohui Ou; Fangping Ouyang; Lifu Zhang; Wenjing Zhang

doi:10.1039/d3nh00159h

Pt single atoms meet metal-organic frameworks to enhance electrocatalytic hydrogen evolution activity

Nanoscale Horiz. 2023 Aug 21;8(9):1273-1281. doi: 10.1039/d3nh00159h.

Authors

Jingting Zhu^{1

2

3}, Yingqian Cen^{1

2}, Haibin Ma³, Weiguang Lian^{1

2}, Jidong Liu^{1

2}, Haohui Ou^{1

2}, Fangping Ouyang⁴, Lifu Zhang^{1

2}, Wenjing Zhang^{1

2}

Affiliations

¹ State Key Laboratory of Radio Frequency Heterogeneous Integration, Shenzhen University, Shenzhen 518060, China. wjzhang@szu.edu.cn.
² International Collaborative Laboratory of 2D Materials for Optoelectronics Science and Technology of Ministry of Education, Institute of Microscale Optoelectronics, Shenzhen University, Shenzhen 518060, China.
³ SIAMC Advanced Materials Co., Ltd, 313100, Huzhou, China.
⁴ School of Physics and Electronics, Central South University, Changsha 410083, China.

PMID: 37465873
DOI: 10.1039/d3nh00159h

Abstract

The electrochemical hydrogen evolution reaction (HER) effectively produces clean, renewable, and sustainable hydrogen; however, the development of efficient electrocatalysts is required to reduce the high energy barrier of the HER. Herein, we report two excellent single-atom (SA)/metal-organic framework (MOF) composite electrocatalysts (Pt_SA-MIL100(Fe) and Pt_SA-MIL101(Cr)) for HER. The obtained Pt_SA-MIL100(Fe) and Pt_SA-MIL101(Cr) electrocatalysts exhibit overpotentials of 60 and 61 mV at 10 mA cm^-2, respectively, which are close to that of commercial Pt/C (38 mV); they exhibit overpotentials of 310 and 288 mV at 200 mA cm^-2, respectively, which are comparable to that of commercial Pt/C (270 mV). Theoretical simulations reveal that Pt SAs modulate the electronic structures of the MOFs, leading to the optimization of the binding strength for H* and significant enhancement of the HER activity. This study describes a novel strategy for preparing desirable HER electrocatalysts based on the synergy between SAs and MIL-series MOFs. Using MIL-series MOFs to support SAs could be valuable for future catalyst design.