{"title":"Enhancing Benzylamine Electro-Oxidation and Hydrogen Evolution Through in-situ Electrochemical Activation of CoC2O4 Nanoarrays","authors":"Guanqiao Zhang, Jialai Hu, Wanling Zhang, Kun Yu, Wenbiao Zhang, Qingsheng Gao","doi":"10.1002/cssc.202401446","DOIUrl":null,"url":null,"abstract":"<p>The sluggish anodic oxygen evolution reaction (OER) seriously restricts the overall efficiency of water splitting. Here, we present an environmentally friendly and efficient aniline oxidation (BOR) to replace the sluggish OER, accomplishing the co-production of H<sub>2</sub> and high value-added benzonitrile (BN) at low voltages. Cobalt oxalates grown on cobalt foam (CoC<sub>2</sub>O<sub>4</sub> ⋅ 2H<sub>2</sub>O/CF) are adopted as the pre-catalysts, which further evolve into working electrocatalysts active for BOR and HER via appropriate electrochemical activation. Thereinto, cyclic voltammetry activation at positive potentials is performed to reconstruct cobalt oxalate via extensive oxidation, resulting in enriched Co(III) species and nanoporous structures beneficial for BOR, while chronoamperometry at negative potentials is introduced for the cathodic activation toward efficient HER with obvious improvement. The two activated electrodes can be combined into a two-electrode system, which achieves a high current density of 75 mA cm<sup>−2</sup> at the voltage of 1.95 V, with the high Faraday efficiencies of both BOR (90.0 %) and HER (90.0 %) and the satisfactory yield of BN (76.8 %).</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":"18 2","pages":""},"PeriodicalIF":7.5000,"publicationDate":"2024-08-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"ChemSusChem","FirstCategoryId":"92","ListUrlMain":"https://onlinelibrary.wiley.com/doi/10.1002/cssc.202401446","RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
引用次数: 0
Abstract
The sluggish anodic oxygen evolution reaction (OER) seriously restricts the overall efficiency of water splitting. Here, we present an environmentally friendly and efficient aniline oxidation (BOR) to replace the sluggish OER, accomplishing the co-production of H2 and high value-added benzonitrile (BN) at low voltages. Cobalt oxalates grown on cobalt foam (CoC2O4 ⋅ 2H2O/CF) are adopted as the pre-catalysts, which further evolve into working electrocatalysts active for BOR and HER via appropriate electrochemical activation. Thereinto, cyclic voltammetry activation at positive potentials is performed to reconstruct cobalt oxalate via extensive oxidation, resulting in enriched Co(III) species and nanoporous structures beneficial for BOR, while chronoamperometry at negative potentials is introduced for the cathodic activation toward efficient HER with obvious improvement. The two activated electrodes can be combined into a two-electrode system, which achieves a high current density of 75 mA cm−2 at the voltage of 1.95 V, with the high Faraday efficiencies of both BOR (90.0 %) and HER (90.0 %) and the satisfactory yield of BN (76.8 %).
缓慢的阳极氧进化反应(OER)严重限制了水分离的整体效率。在此,我们提出了一种环保高效的苯胺氧化反应(BOR)来替代缓慢的阳极氧进化反应,从而在低电压下实现 H2 和高附加值苯腈(BN)的共生。在泡沫钴(CoC2O4-2H2O/CF)上生长的草酸钴被用作前催化剂,经过适当的电化学活化后,草酸钴进一步演变成对 BOR 和 HER 有活性的工作电催化剂。其中,在正电位下进行循环伏安法活化,通过广泛的氧化作用重建草酸钴,从而产生丰富的 Co(III)物种和有利于 BOR 的纳米多孔结构;而在负电位下引入计时跃迁法进行阴极活化,从而明显改善高效 HER。两个活化电极可组合成一个双电极系统,在 1.95 V 的电压下可达到 75 mA cm-2 的高电流密度,同时具有较高的 BOR(90.0%)和 HER(90.0%)法拉第效率,以及令人满意的 BN 产量(76.8%)。
期刊介绍:
ChemSusChem
Impact Factor (2016): 7.226
Scope:
Interdisciplinary journal
Focuses on research at the interface of chemistry and sustainability
Features the best research on sustainability and energy
Areas Covered:
Chemistry
Materials Science
Chemical Engineering
Biotechnology