{"title":"Pt single atoms on Cu nanowires facilitate anodic hydrogen production through efficient electrochemical formaldehyde oxidation","authors":"Jianghui Qiu, Xiafei Gao, Juan Peng","doi":"10.1016/j.cej.2025.162961","DOIUrl":null,"url":null,"abstract":"The formaldehyde oxidation reaction (FOR) with ultra-low potential is an ideal alternative to the oxygen evolution reaction (OER), significantly reducing hydrogen production energy consumption. This reaction not only generates high-value formic acid but also releases H<sub>2</sub> at low potential, enhancing hydrogen production efficiency and economic viability. However, developing efficient and low-cost electrocatalysts remains a key challenge. In this study, a Pt single atom on Cu nanowire catalyst shows high catalytic activity for formaldehyde oxidation reaction (FOR). The catalyst achieves a current density of 100 mA cm<sup>−2</sup> at 0.09 V vs. RHE, with formic acid yield, selectivity, and formaldehyde conversion rate all close to 100 %. A bipolar hydrogen production system (FOR-HER) based on Pt<sub>SA</sub>-Cu NWs and Pt/C assembly achieves a current density of 100 mA cm<sup>−2</sup> at a low cell voltage of 0.12 V, demonstrating a Faraday efficiency close to 100 % for H<sub>2</sub> at both the anode and cathode, and can stable operation for 30 h. Density functional theory (DFT) studies reveal that the interaction between Pt single atoms and Cu enhances hydrogen adsorption, significantly reducing the free energy of H* coupling and thereby improving hydrogen production efficiency. This study elucidates the intrinsic mechanism behind the enhanced performance, providing valuable guidance for the development of high-performance, low-cost single-atom catalysts.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"108 1","pages":""},"PeriodicalIF":13.2000,"publicationDate":"2025-04-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Chemical Engineering Journal","FirstCategoryId":"5","ListUrlMain":"https://doi.org/10.1016/j.cej.2025.162961","RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"ENGINEERING, CHEMICAL","Score":null,"Total":0}
引用次数: 0
Abstract
The formaldehyde oxidation reaction (FOR) with ultra-low potential is an ideal alternative to the oxygen evolution reaction (OER), significantly reducing hydrogen production energy consumption. This reaction not only generates high-value formic acid but also releases H2 at low potential, enhancing hydrogen production efficiency and economic viability. However, developing efficient and low-cost electrocatalysts remains a key challenge. In this study, a Pt single atom on Cu nanowire catalyst shows high catalytic activity for formaldehyde oxidation reaction (FOR). The catalyst achieves a current density of 100 mA cm−2 at 0.09 V vs. RHE, with formic acid yield, selectivity, and formaldehyde conversion rate all close to 100 %. A bipolar hydrogen production system (FOR-HER) based on PtSA-Cu NWs and Pt/C assembly achieves a current density of 100 mA cm−2 at a low cell voltage of 0.12 V, demonstrating a Faraday efficiency close to 100 % for H2 at both the anode and cathode, and can stable operation for 30 h. Density functional theory (DFT) studies reveal that the interaction between Pt single atoms and Cu enhances hydrogen adsorption, significantly reducing the free energy of H* coupling and thereby improving hydrogen production efficiency. This study elucidates the intrinsic mechanism behind the enhanced performance, providing valuable guidance for the development of high-performance, low-cost single-atom catalysts.
超低电位甲醛氧化反应(FOR)是一种理想的析氧反应(OER)替代品,可显著降低制氢能耗。该反应不仅能生成高值甲酸,还能以低电位释放氢气,提高制氢效率和经济可行性。然而,开发高效、低成本的电催化剂仍然是一个关键的挑战。在本研究中,铂单原子铜纳米线催化剂对甲醛氧化反应(for)表现出较高的催化活性。在0.09 V / RHE条件下,催化剂的电流密度为100 mA cm−2,甲酸收率、选择性和甲醛转化率均接近100% %。基于PtSA-Cu NWs和Pt/C组件的双极制氢系统(for - her)在0.12 V的低电池电压下实现了100 mA cm - 2的电流密度,显示出H2在阳极和阴极的法拉第效率接近100% %,并且可以稳定运行30 h。密度泛函理论(DFT)研究表明,Pt单原子与Cu之间的相互作用增强了氢的吸附,显著降低了H*偶联的自由能,从而提高了制氢效率。该研究阐明了性能增强背后的内在机制,为开发高性能、低成本的单原子催化剂提供了有价值的指导。
期刊介绍:
The Chemical Engineering Journal is an international research journal that invites contributions of original and novel fundamental research. It aims to provide an international platform for presenting original fundamental research, interpretative reviews, and discussions on new developments in chemical engineering. The journal welcomes papers that describe novel theory and its practical application, as well as those that demonstrate the transfer of techniques from other disciplines. It also welcomes reports on carefully conducted experimental work that is soundly interpreted. The main focus of the journal is on original and rigorous research results that have broad significance. The Catalysis section within the Chemical Engineering Journal focuses specifically on Experimental and Theoretical studies in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. These studies have industrial impact on various sectors such as chemicals, energy, materials, foods, healthcare, and environmental protection.