Oxygen-rich ligands tailored for novel metal-organic gel electrocatalyst to promote two-electron selectivity electrocatalysis

Xinghao Zhang; Chen Li; Haikuo Lan; Yang Liu; Huihui Zhao; Min Yuan; Yuzhuang Song; Shaoxiang Li; Lei Wang; Kang Liu

doi:10.1016/j.jcis.2022.05.149

Oxygen-rich ligands tailored for novel metal-organic gel electrocatalyst to promote two-electron selectivity electrocatalysis

J Colloid Interface Sci. 2022 Oct 15:624:100-107. doi: 10.1016/j.jcis.2022.05.149. Epub 2022 May 29.

Authors

Xinghao Zhang¹, Chen Li¹, Haikuo Lan¹, Yang Liu¹, Huihui Zhao¹, Min Yuan¹, Yuzhuang Song¹, Shaoxiang Li², Lei Wang³, Kang Liu⁴

Affiliations

¹ Key Laboratory of Eco-chemical Engineering, Taishan Scholar Advantage and Characteristic Discipline Team of Eco-Chemical Process and Technology, College of Chemistry and Molecular Engineering, Qingdao University of Science and Technology, Qingdao 266042, China.
² College of Environment and Safety Engineering, Qingdao University of Science and Technology, Qingdao 266042, China.
³ Key Laboratory of Eco-chemical Engineering, Taishan Scholar Advantage and Characteristic Discipline Team of Eco-Chemical Process and Technology, College of Chemistry and Molecular Engineering, Qingdao University of Science and Technology, Qingdao 266042, China; College of Environment and Safety Engineering, Qingdao University of Science and Technology, Qingdao 266042, China. Electronic address: inorchemwl@126.com.
⁴ Key Laboratory of Eco-chemical Engineering, Taishan Scholar Advantage and Characteristic Discipline Team of Eco-Chemical Process and Technology, College of Chemistry and Molecular Engineering, Qingdao University of Science and Technology, Qingdao 266042, China; Chaofeng Steel Structure Group Co., Ltd., Hangzhou 311215, China. Electronic address: liukang82@126.com.

PMID: 35660879
DOI: 10.1016/j.jcis.2022.05.149

Abstract

More extensive attention has been garnered about the H₂O₂ electroproduction via two-electron oxygen reduction reaction (2e^- ORR). Aiming to develop a more active, more selective and more stable catalyst, herein we reported an unconventional raw metal-organic gels (MOGs) toward this process. This pioneering work, by ingeniously designing and altering the precursor ligands, achieving precisely controlling the number of oxygen groups (OGs). By elaborately comparing more than 70 samples, uncovered the significance that OGs could sufficiently promote the selectivity for H₂O₂ electrochemical synthesis through the two-electron pathway (realizing enhancement more than 20% in this work). The most potential Fe_0.1Co_0.9 MOG (H₆L), performing an onset potential of 0.76 V (low overpotential), a high selectivity up to 93% ranging 0.15 V to 0.65 V (large voltage window) and 2.1 electron transfer number (implying the 2e^- process dominate). This study, unlike other oxidation treatment, through the precise regulation of precursors, further confirmed the feasibility of oxygen-containing functional groups (OGs) tailoring strategy, providing a possibility for low-cost and efficient potential candidate of 2e^- ORR.

Keywords: 2e(-) ORR; H(2)O(2) selectivity; Metal–organic gel; OGs; Precursor design.