电催化OER用过渡金属-硫族化物修饰碳纳米管的局部石墨化

IF 7.9 3区 材料科学 Q1 GREEN & SUSTAINABLE SCIENCE & TECHNOLOGY
Thibault De Villenoisy , Yue Jiang , Xiaoran Zheng , Yihao Shan , Calvin Hoang , Vienna Wong , Leigh Sheppard , Pramod Koshy , Charles C. Sorrell , Sajjad S. Mofarah
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引用次数: 0

摘要

为了使可持续生产绿色氢的技术成功商业化,镍基(Ni)和铁基(Fe)材料是最有前途的廉价和有效的无贵金属碱性OER催化剂。采用了一种基于成本效益和高产率的制备策略,在室温下在水溶液中合成了Ni-, Fe-和mo掺杂的ZIF-8 (Zn),例如NiFeMo-ZIF-8作为前驱体。随后,前驱体在惰性气氛(800°C)中(如NiFeMo-C)进行热解碳化,然后在富硫(S)和富磷(P)气氛中进行二次热处理,在导电多孔氮掺杂多壁碳纳米管(N- mwcnts)中(如NiFeMo-C- ps)制备高热力学活性和低浓度过渡金属硫系(TMC)纳米颗粒。结果表明,MWCNTs(直径约10 nm)包裹金属衍生物(MDs),通过高导电性的MWCNTs实现了相当快的电子转移,从而通过(1)最小的扩散途径实现了有效的电荷转移,(2)增加了金属衍生物的可及性,从而根据工作电压下的热气氛和OER电解质中的转换形成不同的活性位点,从而加速了OER性能。催化表面积主要是由Mo和S掺杂剂负载的NiFeOOH,并由磷酸盐离子共催化。性能最好的催化剂是Ni、Fe、mo掺杂的ZIF-8,经热解后在富P、富s气氛中热处理得到NiFeMo-C-PS;结果表明,在1 a cm−2时,塔菲尔斜率为52 mV / dec−1,过电位为437 mV。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
Localized graphitization on transition-metal-chalcogenide-decorated carbon nanotubes for electrocatalytic OER
For successful commercialization of technologies for the sustainable production of green hydrogen, nickel (Ni)- and iron (Fe)-based materials are the most promising cheap and effective noble metal-free catalysts for alkaline OER catalysis. A fabrication strategy was adopted based on a cost-effective and high-yield synthesis of Ni-, Fe-, and Mo-doped ZIF-8 (Zn), e.g. NiFeMo-ZIF-8, as the precursor, in an aqueous solution at room temperature. Subsequently, the precursor was subjected to pyrolysis for carbonization in an inert atmosphere (800 °C), e.g. NiFeMo–C, before secondary thermal treatment in sulfur (S) and phosphorus (P)-rich atmospheres to produce highly thermodynamically-active and low concentration transition metal chalcogenide (TMC) nanoparticles in conductive and porous nitrogen (N)-doped multiwalled-carbon-nanotubes (N-MWCNTs), e.g. NiFeMo-C-PS. The results revealed that the wrapping of the metal derivatives (MDs) by the MWCNTs (∼10 nm diameter) resulted in considerably rapid electron transfer via the highly conductive MWCNTs, leading to accelerated OER performance through (1) minimal diffusion pathways which enabled efficient charge transfer and (2) the increased accessibility of metal derivatives, which formed varying active sites depending on the thermal atmosphere and conversion in the OER electrolyte at the operating voltage. The catalytic surface area was determined to be primarily NiFeOOH supported by Mo and S dopants with co-catalysis from phosphate ions. The best performing catalyst was Ni,Fe,Mo-doped ZIF-8 that was pyrolyzed and then heat treated in a P- and S-rich atmosphere to produce NiFeMo-C-PS; this showed a Tafel slope of 52 mV dec−1 and overpotential of 437 mV at 1 A cm−2.
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来源期刊
CiteScore
5.80
自引率
6.40%
发文量
174
审稿时长
32 days
期刊介绍: Materials Today Sustainability is a multi-disciplinary journal covering all aspects of sustainability through materials science. With a rapidly increasing population with growing demands, materials science has emerged as a critical discipline toward protecting of the environment and ensuring the long term survival of future generations.
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