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Rh2S3/N‐Doped Carbon Hybrids as pH‐Universal Bifunctional Electrocatalysts for Energy‐Saving Hydrogen Evolution
Small Methods ( IF 10.7 ) Pub Date : 2020-05-25 , DOI: 10.1002/smtd.202000208
Chaoxiong Zhang 1, 2 , Haoxuan Liu 2 , Yifan Liu 3 , Xijun Liu 2 , Yuying Mi 2 , Ruijie Guo 2 , Jiaqiang Sun 4 , Haihong Bao 2 , Jia He 2 , Yuan Qiu 2 , Junqiang Ren 5 , Xiangjun Yang 1 , Jun Luo 2 , Guangzhi Hu 1
Affiliation  

Using hydrazine oxidation reaction (HzOR) to replace the oxygen evolution reaction is an effective way to decrease the overpotential of the anodic reaction in overall water splitting (OWS), facilitating cost‐effective and safe hydrogen production. Herein, Rh2S3/N‐doped carbon hybrids (Rh2S3/NC) are first reported as novel and efficient bifunctional electrocatalysts for hydrazine‐assisted hydrogen generation over a wide pH range. Specifically, Rh2S3/NC exhibits low overpotentials for the hydrogen evolution reaction (HER) in alkaline (38 mV), neutral (46 mV), and acidic (21 mV) electrolytes, to reach the current density of 10 mA cm−2, and maintains the activities over 70 h. Meanwhile, Rh2S3/NC also displays competitive HzOR performance at all‐pH electrolytes. Thus, serving as a bifunctional electrocatalyst for both HER and HzOR, Rh2S3/NC shows overwhelming‐Pt/C performance in three electrolytes, and can save over 93.3%, 85.2%, and 78.3% energy consumption compared to the corresponding OWS system. Moreover, theoretical calculations confirm that Rh2S3/NC owns low free‐energy changes of the H adsorption and the dehydrogenation of adsorbed NHNH both of which are beneficial to enhance catalytic activity. This work develops a novel bifunctional electrocatalyst with free pH‐dependent condition for the hydrazine‐assisted electrolysis system to furtherly reduce the cost of massive industrial H2 production.

中文翻译:

Rh2S3 / N掺杂的碳杂化物作为pH通用的双功能电催化剂,可节省氢气

使用肼氧化反应(HzOR)代替氧气释放反应是减少整体水分解(OWS)中阳极反应过电位的有效方法,从而促进了经济高效且安全的制氢。在此,Rh 2 S 3 / N掺杂的碳杂化物(Rh 2 S 3 / NC)首次被报道为在宽pH范围内肼辅助制氢的新型高效双功能电催化剂。具体而言,铑2小号3 / NC显示出低的超电势在碱性(38毫伏)的氢生成反应(HER),中性(46毫伏),和酸性(21毫伏)的电解质,到达的10毫安厘米的电流密度- 2,并维持超过70小时的活动。同时,Rh 2 S 3 / NC在全pH电解液中也显示出极好的HzOR性能。因此,Rh 2 S 3 / NC用作HER和HzOR的双功能电催化剂,在三种电解液中表现出压倒性的Pt / C性能,与相应的OWS相比可节省93.3%,85.2%和78.3%的能耗。系统。此外,理论计算证实Rh 2 S 3/ NC具有较低的H吸附自由能变化和NHNH吸附脱氢,这都有助于增强催化活性。这项工作开发了一种新型的具有游离pH依赖性条件的双功能电催化剂,用于肼辅助电解系统,以进一步降低大规模工业H 2的生产成本。
更新日期:2020-05-25
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