Chemically Robust, Cu-based Porous Coordination Polymer Nanosheets for Efficient Hydrogen Evolution: Experimental and Theoretical Studies

Bihang Zhou; Jia-Jia Zheng; Jingui Duan; Chunchao Hou; Yang Wang; Wanqin Jin; Qiang Xu

doi:10.1021/acsami.9b04471

Chemically Robust, Cu-based Porous Coordination Polymer Nanosheets for Efficient Hydrogen Evolution: Experimental and Theoretical Studies

ACS Appl Mater Interfaces. 2019 Jun 12;11(23):21086-21093. doi: 10.1021/acsami.9b04471. Epub 2019 May 28.

Authors

Bihang Zhou¹, Jia-Jia Zheng^{2

3}, Jingui Duan¹, Chunchao Hou⁴, Yang Wang¹, Wanqin Jin¹, Qiang Xu⁴

Affiliations

¹ State Key Laboratory of Materials-Oriented Chemical Engineering, College of Chemical Engineering , Nanjing Tech University , Nanjing 211800 , China.
² Institute for Integrated Cell-Material Sciences , Kyoto University , Yoshida , Sakyo-ku, Kyoto 606-8501 , Japan.
³ Fukui Institute for Fundamental Chemistry , Kyoto University , Nishi-hiraki cho, Takano , Sakyo-ku, Kyoto 606-8103 , Japan.
⁴ National Institute of Advanced Industrial Science and Technology-Kyoto University Chemical Energy Materials Open Innovation Laboratory , Yoshida , Sakyo-Ku, Kyoto 606-8501 , Japan.

PMID: 31091075
DOI: 10.1021/acsami.9b04471

Abstract

Due to the extremely high number of accessible active sites and short diffusion path, porous coordination polymer (PCP) nanosheets have demonstrated a variety of promising applications, especially for energy conversion and mass transfer. However, the development of chemically stable PCP nanosheets with dense active sites and large lateral size is a great challenge in terms of feasible considerations. Herein, we first designed and prepared a kind of chemically stable PCP nanosheets via a bottom-up and a top-down integral strategy. Featuring densely exposed and periodic Cu²⁺ active sites (2.1 × 10⁶ per μm²), as well as ultrathin nature (5 nm) and significant pores (18 Å), this nanosheet demonstrated remarkable performance of electrocatalytic hydrogen evolution. Furthermore, one plausible process and the effect of Cu²⁺ active sites were proposed and validated by density functional theory calculations.

Keywords: Cu active site; chemical stability; electrocatalytic hydrogen evolution; mechanism study; porous coordination polymer design; ultrathin layer.