Interfacial carbon dots introduced distribution-structure modulation of Pt loading on graphene towards enhanced electrocatalytic hydrogen evolution reaction

He Xiao; Meng Bai; Man Zhao; Zimei Fu; Wenxiang Wang; Peipei Zhao; Jiamin Ma; Li Zhang; Junming Zhang; Yingluo He; Jian Zhang; Jianfeng Jia

doi:10.1016/j.jcis.2023.11.102

Interfacial carbon dots introduced distribution-structure modulation of Pt loading on graphene towards enhanced electrocatalytic hydrogen evolution reaction

J Colloid Interface Sci. 2024 Feb 15:656:214-224. doi: 10.1016/j.jcis.2023.11.102. Epub 2023 Nov 19.

Authors

He Xiao¹, Meng Bai¹, Man Zhao², Zimei Fu¹, Wenxiang Wang¹, Peipei Zhao¹, Jiamin Ma¹, Li Zhang¹, Junming Zhang¹, Yingluo He³, Jian Zhang⁴, Jianfeng Jia⁵

Affiliations

¹ Key Laboratory of Magnetic Molecules & Magnetic Information Materials Ministry of Education, The School of Chemical and Material Science, Shanxi Normal University, Taiyuan 030000, China.
² Key Laboratory of Magnetic Molecules & Magnetic Information Materials Ministry of Education, The School of Chemical and Material Science, Shanxi Normal University, Taiyuan 030000, China. Electronic address: zm03030225@sxnu.edu.cn.
³ Department of Applied Chemistry, School of Engineering, University of Toyama, Gofuku 3190, Toyama 930-8555, Japan.
⁴ State Key Laboratory of Solidification Processing and School of Materials Science and Engineering, Northwestern Polytechnical University, Xi'an, Shaanxi 710072, China. Electronic address: zhangjian@nwpu.edu.cn.
⁵ Key Laboratory of Magnetic Molecules & Magnetic Information Materials Ministry of Education, The School of Chemical and Material Science, Shanxi Normal University, Taiyuan 030000, China. Electronic address: jiajf@dns.sxnu.edu.cn.

PMID: 37989054
DOI: 10.1016/j.jcis.2023.11.102

Abstract

To easily load Pt on smoothy graphene synthesized by cathodic exfoliation method and achieve adjacent plane distribution of Pt, carbon dots (CDs) are used to construct anchoring points to load highly dispersed Pt species due to strong interaction between CDs and Pt species. The composite of Pt-CDs/graphene is synthesized via a continuous process of cathodic exfoliation-hydrothermal-impregnation-reduction. Characterization results indicate the distribution configuration of Pt varies from coated structure of CDs@Pt to dispersed configuration of CDs&Pt or Pt&CDs, then to wrapping configuration of Pt@CDs with increased amount of CDs. It's found that suitable introduction of CDs promotes the adjacent plane distribution of Pt species. The obtained best Pt-4CDs/G shows the low overpotential of 36 mV (10 mA⋅cm^-2) and high mass activity of 3747.8 mA mg^-1 at -40 mV towards electrocatalytic hydrogen evolution reaction (HER), 9.2 times more active than that of Pt/C (406.2 mA mg^-1). The superior HER performance of Pt-4CDs/G is attributed to its relatively adjacent plane distribution of Pt, which supports high electrochemically active surface area and more adjacent Pt sites for H* adsorption. Benefitting from that, the HER process for Pt-4CDs/G favorably follows the Tafel pathway, resulting in low hydrogen adsorption free energy and excellent HER activity.

Keywords: Carbon dot; Distribution-structure; Hydrogen evolution reaction; Pt.