{"title":"电子再分布对氢吸附和制氢效率的影响","authors":"Wansheng Ruan, Yiran Teng, Hanming Zhang, Zhihui Li, Tongguang Xu, Yalin Yang, Fei Teng","doi":"10.1016/j.mtchem.2024.102244","DOIUrl":null,"url":null,"abstract":"Water electrolysis is a promising, carbonless technology for hydrogen production, however, its widely industrial application is severely limited by the extensive energy consumption caused by sluggish oxygen evolution reaction (OER) kinetics. Herein, the simple Mn doping is employed to finely tune sulfur vacancies (V). The thoeretic calculations prove that the electron structure has been well controlled. Compared with perfect MoS (without V), the electron re-distribution of Mn-doped MoS with V (Vs-Mn-MoS) exhibits the both modes: electron depletion near the V and electron accumulation between two Mo atoms. Furthermore, the well-controlled electron structure obviously promotes H adsorption. The experimental results shows that the 5 wt% Mn–MoS exhibits an excellent hydrogen evolution reaction (HER) activity (79 mV/10 mA cm, 55.46 mV dec), which is better than the other MoS-based electrolysts in the previous reports. Moreover, an innovative substitution anode reaction is designed, namely, glycerol oxidation reaction (GOR)-based symmetric electrolyser with Mn–MoS as the both electrodes. At 60 mA cm, the cell voltage of GOR-based electrolyser has decreased by 14.8 %, and its Faradaic efficiency for HER increases by 10.04 % compared to conventional water-based one. This result proves that about 14.8 % of electric energy can be economized. Thus, this innovative electrocatalysis system could be promising for industrial hydrogen production.","PeriodicalId":18353,"journal":{"name":"Materials Today Chemistry","volume":"19 1","pages":""},"PeriodicalIF":6.7000,"publicationDate":"2024-08-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Effect of electron redistribution on H adsorption and hydrogen production efficiency\",\"authors\":\"Wansheng Ruan, Yiran Teng, Hanming Zhang, Zhihui Li, Tongguang Xu, Yalin Yang, Fei Teng\",\"doi\":\"10.1016/j.mtchem.2024.102244\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"Water electrolysis is a promising, carbonless technology for hydrogen production, however, its widely industrial application is severely limited by the extensive energy consumption caused by sluggish oxygen evolution reaction (OER) kinetics. Herein, the simple Mn doping is employed to finely tune sulfur vacancies (V). The thoeretic calculations prove that the electron structure has been well controlled. Compared with perfect MoS (without V), the electron re-distribution of Mn-doped MoS with V (Vs-Mn-MoS) exhibits the both modes: electron depletion near the V and electron accumulation between two Mo atoms. Furthermore, the well-controlled electron structure obviously promotes H adsorption. The experimental results shows that the 5 wt% Mn–MoS exhibits an excellent hydrogen evolution reaction (HER) activity (79 mV/10 mA cm, 55.46 mV dec), which is better than the other MoS-based electrolysts in the previous reports. Moreover, an innovative substitution anode reaction is designed, namely, glycerol oxidation reaction (GOR)-based symmetric electrolyser with Mn–MoS as the both electrodes. At 60 mA cm, the cell voltage of GOR-based electrolyser has decreased by 14.8 %, and its Faradaic efficiency for HER increases by 10.04 % compared to conventional water-based one. This result proves that about 14.8 % of electric energy can be economized. Thus, this innovative electrocatalysis system could be promising for industrial hydrogen production.\",\"PeriodicalId\":18353,\"journal\":{\"name\":\"Materials Today Chemistry\",\"volume\":\"19 1\",\"pages\":\"\"},\"PeriodicalIF\":6.7000,\"publicationDate\":\"2024-08-14\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Materials Today Chemistry\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://doi.org/10.1016/j.mtchem.2024.102244\",\"RegionNum\":2,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Materials Today Chemistry","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1016/j.mtchem.2024.102244","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
摘要
水电解是一种前景广阔的无碳制氢技术,但由于氧进化反应(OER)动力学缓慢,导致能耗过大,从而严重限制了其在工业上的广泛应用。本文采用简单的锰掺杂来微调硫空位(V)。热力学计算证明,电子结构得到了很好的控制。与完美的 MoS(不含 V)相比,掺有锰的 MoS(Vs-Mn-MoS)的电子再分布表现出两种模式:V 附近的电子耗尽和两个 Mo 原子间的电子积聚。此外,良好的电子结构明显促进了 H 的吸附。实验结果表明,5 wt% 的锰-MoS 具有优异的氢进化反应(HER)活性(79 mV/10 mA cm, 55.46 mV dec),优于之前报道的其他 MoS 基电解质。此外,还设计了一种创新的置换阳极反应,即以 Mn-MoS 为两极的基于甘油氧化反应(GOR)的对称电解槽。与传统的水基电解槽相比,在 60 mA cm 的条件下,甘油氧化反应电解槽的电池电压降低了 14.8%,其 HER 的法拉第效率提高了 10.04%。这一结果证明可以节省约 14.8% 的电能。因此,这种创新的电催化系统在工业制氢方面大有可为。
Effect of electron redistribution on H adsorption and hydrogen production efficiency
Water electrolysis is a promising, carbonless technology for hydrogen production, however, its widely industrial application is severely limited by the extensive energy consumption caused by sluggish oxygen evolution reaction (OER) kinetics. Herein, the simple Mn doping is employed to finely tune sulfur vacancies (V). The thoeretic calculations prove that the electron structure has been well controlled. Compared with perfect MoS (without V), the electron re-distribution of Mn-doped MoS with V (Vs-Mn-MoS) exhibits the both modes: electron depletion near the V and electron accumulation between two Mo atoms. Furthermore, the well-controlled electron structure obviously promotes H adsorption. The experimental results shows that the 5 wt% Mn–MoS exhibits an excellent hydrogen evolution reaction (HER) activity (79 mV/10 mA cm, 55.46 mV dec), which is better than the other MoS-based electrolysts in the previous reports. Moreover, an innovative substitution anode reaction is designed, namely, glycerol oxidation reaction (GOR)-based symmetric electrolyser with Mn–MoS as the both electrodes. At 60 mA cm, the cell voltage of GOR-based electrolyser has decreased by 14.8 %, and its Faradaic efficiency for HER increases by 10.04 % compared to conventional water-based one. This result proves that about 14.8 % of electric energy can be economized. Thus, this innovative electrocatalysis system could be promising for industrial hydrogen production.
期刊介绍:
Materials Today Chemistry is a multi-disciplinary journal dedicated to all facets of materials chemistry.
This field represents one of the fastest-growing areas of science, involving the application of chemistry-based techniques to the study of materials. It encompasses materials synthesis and behavior, as well as the intricate relationships between material structure and properties at the atomic and molecular scale. Materials Today Chemistry serves as a high-impact platform for discussing research that propels the field forward through groundbreaking discoveries and innovative techniques.