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Co–N-doped single-crystal V3S4 nanoparticles as pH-universal electrocatalysts for enhanced hydrogen evolution reaction
Electrochimica Acta ( IF 6.6 ) Pub Date : 2020-01-13 , DOI: 10.1016/j.electacta.2020.135696
Liyun Cao , Linlin Wang , Liangliang Feng , Jae-hyun Kim , Yingying Du , Dan Yang , Lingjiang Kou , Jianfeng Huang

The exploitation of innovative and high-efficiency inexpensive electrocatalysts for hydrogen evolution reaction (HER) over a wide pH range is highly pivotal but still challenging. Herein, a simple one-step vacuum pyrolysis approach without using H2S is reported to synthesize Co–N-doped single-crystal V3S4 nanoparticles (Co–N–V3S4), which can function as highly active and stable nonprecious electrocatalysts toward HER at all pH values (pH 0–14). Furthermore, we demonstrate that the use of trithiocyanuric acid as both nitrogen and sulfur sources along with Co-precursor can not only trigger the incorporation of highly active Co–N sites and the high-content N doping, but also well modulate its electronic structure and thus the improved electrocatalytic HER activity. Results show that the as-obtained Co–N–V3S4 material needs small overpotentials of 268 mV, 260 mV and 252 mV at the current density of 10 mA cm−2 in acid (pH 0), neutral (pH 7) and alkaline (pH 14) solutions, respectively, and offers a durable catalytic stability for at least 10 h, as well as gives a Faradaic yield close to 100% at all pH values. Our findings of identifying V3S4 as the catalytically active vanadium sulfide phase for HER and developing a metal-doping induced structure-regulating strategy for the enhancement of catalytic performance broaden our horizons and meanwhile provide fresh insights to rationally design highly efficient noble-metal-free electrocatalysts toward water splitting.



中文翻译:

Co-N掺杂单晶V 3 S 4纳米粒子作为pH通用的电催化剂,可增强氢的释放反应

在宽的pH范围内开发用于氢气析出反应(HER)的新颖,高效,廉价的电催化剂是至关重要的,但仍具有挑战性。在此,据报道一种不使用H 2 S的简单的一步热解方法就可以合成掺有Co-N的单晶V 3 S 4纳米颗粒(Co-N-V 3 S 4),在所有pH值(pH 0-14)时,都可作为对HER的高活性和稳定的非贵金属电催化剂。此外,我们证明了使用三硫氰尿酸作为氮源和硫源以及Co前驱体不仅可以触发高活性Co-N位点的掺入和高含量N掺杂,还可以很好地调节其电子结构和因此改善了电催化HER活性。结果表明,所获得的Co–N–V 3 S 4材料在10 mA cm -2的电流密度下需要268 mV,260 mV和252 mV的小过电位。分别在酸(pH 0),中性(pH 7)和碱性(pH 14)溶液中溶解,并提供至少10小时的持久催化稳定性,并且在所有pH值下法拉第收率均接近100%。我们的发现将V 3 S 4鉴定为HER的催化活性硫化钒相,并开发了金属掺杂诱导的结构调节策略以增强催化性能,拓宽了我们的视野,同时也为合理设计高效贵金属提供了新的见解。不含电的催化剂用于水分解。

更新日期:2020-01-13
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