Precious-Metal-Free Electrocatalysts for Activation of Hydrogen Evolution with Nonmetallic Electron Donor: Chemical Composition Controllable Phosphorous Doped Vanadium Carbide MXene

Yoon Yeoheung; Tiwari Anand P.; Choi Min; Novak Travis C.; Song Wooseok; Chang Hyunju; Zyung Taehyoung; Lee Sun Sook; Jeon Seokwoo; An Ki-Seok

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Precious-Metal-Free Electrocatalysts for Activation of Hydrogen Evolution with Nonmetallic Electron Donor: Chemical Composition Controllable Phosphorous Doped Vanadium Carbide MXene

机译：非金属电子给体活化氢释放的无金属无电催化剂：化学成分可控的磷掺杂碳化钒MXene

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The insufficient strategies to improve electronic transport, the poor intrinsic chemical activities, and limited active site densities are all factors inhibiting MXenes from their electrocatalytic applications in terms of hydrogen production. Herein, these limitations are overcome by tunable interfacial chemical doping with a nonmetallic electron donor, i.e., phosphorization through simple heat. treatment with triphenyl phosphine (TPP) as a phosphorous source in 2D vanadium carbide MXene. Through this process, substitution, and/or doping of phosphorous occurs at the basal plane with controllable chemical compositions (3.83-4.84 at%). Density functional theory (DFT) calculations demonstrate that the P-C bonding shows the lowest surface formation energy (Delta G(surf)) of 0.027 eV angstrom(-2) and Gibbs free energy (Delta G(H)) of -0.02 eV, whereas others such as P-oxide and P-V (phosphide) show highly positive Delta G(H). The P3-V2CTx treated at 500 degrees C shows the highest concentration of P-C bonds, and exhibits the lowest onset overpotential of-28 mV, Tafel slope of 74 mV dec(-1), and the smallest overpotential of-163 mV at 10 mA cm(-2) in 0.5 M H2SO4. The first strategy for electrocatalytically accelerating hydrogen evolution activity of V2CTx MXene by simple interfacial doping will open the possibility of manipulating the catalytic performance of various MXenes.

机译：改善电子传输的策略不足，固有的化学活性差以及活性位点密度有限，所有这些都是在生产氢方面抑制MXenes进行电催化应用的因素。在此，通过用非金属电子给体进行可调谐的界面化学掺杂，即通过简单的加热使磷化，克服了这些限制。用三苯基膦（TPP）作为2D碳化钒MXene中的磷源进行处理。通过该过程，在基面上以可控制的化学成分（3.83-4.84 at％）发生磷的取代和/或掺杂。密度泛函理论（DFT）计算表明，PC键合显示出最低的表面形成能（Delta G（surf））为0.027 eV埃（-2），吉布斯自由能（Delta G（H））为-0.02 eV，而P-氧化物和PV（磷化物）等其他化合物则显示出高度正的Delta G（H）。在500摄氏度下处理的P3-V2CTx表现出最高的PC键浓度，并且在10 mA电流下表现出最低的-28 mV起始超电势，74 mV dec（-1）的Tafel斜率和-163 mV的最小超电势在0.5 M H2SO4中的cm（-2）。通过简单的界面掺杂电催化加速V2CTx MXene的氢释放活性的第一种策略将为操纵各种MXene的催化性能提供可能性。

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《Advanced Functional Materials》 |2019年第30期|1903443.1-1903443.12|共12页
作者
Yoon Yeoheung; Tiwari Anand P.; Choi Min; Novak Travis C.; Song Wooseok; Chang Hyunju; Zyung Taehyoung; Lee Sun Sook; Jeon Seokwoo; An Ki-Seok;
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Korea Res Inst Chem Technol, Thin Film Mat Res Ctr, Yuseong POB 107, Daejeon 34114, South Korea;

Korea Adv Inst Sci & Technol, Dept Mat Sci & Engn, Deajeon 34141, South Korea;

Korea Res Inst Chem Technol, Chem Data Driven Res Ctr, Yuseong POB 107, Daejeon 34114, South Korea|Ulsan Inst Sci & Technol, Dept Chem, 50 UNIST Gil, Ulsan 44919, South Korea;

Korea Adv Inst Sci & Technol, Dept Mat Sci & Engn, Deajeon 34141, South Korea;

Korea Res Inst Chem Technol, Thin Film Mat Res Ctr, Yuseong POB 107, Daejeon 34114, South Korea;

Korea Res Inst Chem Technol, Chem Data Driven Res Ctr, Yuseong POB 107, Daejeon 34114, South Korea;

Korea Res Inst Chem Technol, Thin Film Mat Res Ctr, Yuseong POB 107, Daejeon 34114, South Korea;

Korea Res Inst Chem Technol, Thin Film Mat Res Ctr, Yuseong POB 107, Daejeon 34114, South Korea;

Korea Adv Inst Sci & Technol, Dept Mat Sci & Engn, Deajeon 34141, South Korea;

Korea Res Inst Chem Technol, Thin Film Mat Res Ctr, Yuseong POB 107, Daejeon 34114, South Korea;

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2D vanadium carbides; hydrogen evolution reaction; MXene; nonmetallic-electron donor; phosphorous-doping;

机译：2D钒碳化物;氢进化反应;MXENE;非金属 - 电子供体;磷掺杂;

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3. Computational Screening of 2D Ordered Double Transition-Metal Carbides (MXenes) as Electrocatalysts for Hydrogen Evolution Reaction [J] . Jin Di, Johnson Luke R., Raman Abhinav S., The journal of physical chemistry, C. Nanomaterials and interfaces . 2020,第19期

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Precious-Metal-Free Electrocatalysts for Activation of Hydrogen Evolution with Nonmetallic Electron Donor: Chemical Composition Controllable Phosphorous Doped Vanadium Carbide MXene

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