Tuning the electronic metal-carbon interactions in Lignin-based carbon-supported ruthenium-based electrocatalysts for enhanced hydrogen evolution reactions

Qichang Wang; Jing Zhao; Xiaoxuan Yang; Jianfei Li; Chunfei Wu; Dekui Shen; Chongbo Cheng; Lian-Hua Xu

doi:10.1016/j.jcis.2024.03.019

Tuning the electronic metal-carbon interactions in Lignin-based carbon-supported ruthenium-based electrocatalysts for enhanced hydrogen evolution reactions

J Colloid Interface Sci. 2024 Jun 15:664:251-262. doi: 10.1016/j.jcis.2024.03.019. Epub 2024 Mar 5.

Authors

Qichang Wang¹, Jing Zhao¹, Xiaoxuan Yang¹, Jianfei Li¹, Chunfei Wu², Dekui Shen³, Chongbo Cheng⁴, Lian-Hua Xu⁵

Affiliations

¹ Key Laboratory of Energy Thermal Conversion and Control of Ministry of Education, School of Energy and Environment, Southeast University, Nanjing, Jiangsu 210096, PR China.
² School of Chemistry and Chemical Engineering, Queen's University Belfast, Belfast BT7 1NN, United Kingdom.
³ Key Laboratory of Energy Thermal Conversion and Control of Ministry of Education, School of Energy and Environment, Southeast University, Nanjing, Jiangsu 210096, PR China. Electronic address: 101011398@seu.edu.cn.
⁴ Engineering Laboratory of Energy System Process Conversion and Emission Reduction Technology of Jiangsu Province, School of Energy & Mechanical Engineering, Nanjing Normal University, Nanjing 210046, PR China. Electronic address: 62125@njnu.edu.cn.
⁵ MOE Key Laboratory of Environmental Remediation and Ecosystem Health, Institute of Environmental Health, College of Environmental and Resource Sciences, Zhejiang University, Hangzhou 310058, PR China. Electronic address: xulianhua@zju.edu.cn.

PMID: 38467090
DOI: 10.1016/j.jcis.2024.03.019

Abstract

Ruthenium (Ru) nanoparticles dispersed on carbon support are promising electrocatalysts for hydrogen evolution reaction (HER) due to strong electronic metal-carbon interactions (EMCIs). Defects engineering in carbon supports is an effective strategy to adjust EMCIs. We prepared nitrogen/sulfur co-doped carbon supported Ru nanoparticles (Ru@N/S-LC) using sodium lignosulfonate and urea as feedstocks. Intrinsic S dopants from sodium lignosulfonate create rich S defects, thus enhancing the EMCIs within Ru@N/S-LC, leading a faster electron transfer between Ru nanoparticles and N/S-LC compared with N-doped carbon supported Ru nanoparticles (Ru@N-CC). The resulting Ru@N/S-LC exhibits an enhanced work function and a down-shifted d-band center, inducing stronger electron capturing ability and weaker hydrogen desorption energy than Ru@N-CC. Ru@N/S-LC requires only 7 and 94 mV overpotential in acidic medium and alkaline medium to achieve a current density of 10 mA cm^-2. Density Functional Theory (DFT) calculations were utilized to clarify the impact of sulfur (S) doping and the mechanism underlying the notable catalytic activity of Ru@N/S-LC. This study offers a perspective for utilizing the natural dopants of biomass to adjust the EMCIs for electrocatalysts.

Keywords: Electronic metal-carbon interactions; Hydrogen evolution reaction; Ruthenium nanoparticles; Sodium lignosulfonate-based carbon; Sulfur defects.