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Two-Dimensional Carbonitride MXenes as an Efficient Electrocatalyst for Hydrogen Evolution
The Journal of Physical Chemistry C ( IF 3.3 ) Pub Date : 2021-02-23 , DOI: 10.1021/acs.jpcc.0c09513 Bo Wei 1, 2 , Zhongheng Fu 1, 2 , Dominik Legut 3 , Timothy C. Germann 4 , Qianfan Zhang 1, 2 , Shiyu Du 5 , Haijun Zhang 6, 7 , Joseph S. Francisco 8 , Ruifeng Zhang 1, 2
The Journal of Physical Chemistry C ( IF 3.3 ) Pub Date : 2021-02-23 , DOI: 10.1021/acs.jpcc.0c09513 Bo Wei 1, 2 , Zhongheng Fu 1, 2 , Dominik Legut 3 , Timothy C. Germann 4 , Qianfan Zhang 1, 2 , Shiyu Du 5 , Haijun Zhang 6, 7 , Joseph S. Francisco 8 , Ruifeng Zhang 1, 2
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Owing to their excellent thermostability, superior electrical conductivity, and tunable surface chemistry, two-dimensional transition-metal carbides, nitrides, and carbonitrides (MXenes) are highly desirable as potential electrocatalysts for the hydrogen evolution reaction (HER). However, while nearly 30 MXenes have already been synthesized, less carbonitride MXenes were experimentally reported so far, yet their potential promising electrochemical properties are greatly expected. Here, we explored the thermodynamically favorable configurations of Mo2(CN)Tx (T = F, OH, and O) with a mixture of functional groups under various electrochemical environments. It is revealed that the O*/OH*-terminated Mo-based carbonitride MXenes exhibit the most stable state under ambient conditions. By exploring the catalytic performance of HER for various Mo2(CxN1–x)T2 at different ratios of C and N atoms, we found that three optimal C/N ratios with 0.5 ML O* and 0.5 ML OH* showed good catalytic activity of HER, comparable to Pt metals. Further investigations of strain-tunable HER of the cofunctionalized Mo2(CxN1–x)OOH suggest that the biaxial strain may effectively modify the ΔGH* of HER, which can be ascribed to the asymmetrical surface topology and charge polarization. These results provide not only a strategy to synthesize carbonitride MXenes with various surface functionalizations but also a feasible solution to design by chemical doping and strain engineering.
中文翻译：
二维碳氮化物MXenes作为氢析出的高效电催化剂
由于其优异的热稳定性，优异的电导率和可调节的表面化学性质，二维过渡金属碳化物，氮化物和碳氮化物（MXenes）非常适合作为氢释放反应（HER）的潜在电催化剂。然而，尽管已经合成了近30种MXene，但到目前为止，实验上报道的碳氮化物MXene较少，但是人们非常希望其潜在的有前途的电化学性能。在这里，我们探讨了Mo 2（CN）T x的热力学有利构型（T = F，OH和O）在各种电化学环境下带有官能团的混合物。结果表明，O * / OH *端基的Mo基碳氮化物MXenes在环境条件下表现出最稳定的状态。通过探索HER在不同的C和N原子比下对各种Mo 2（C x N 1– x）T 2的催化性能，我们发现三个最佳的C / N比为0.5 ML O *和0.5 ML OH * HER的催化活性好于Pt金属。对共官能化的Mo 2（C x N 1– x）OOH的可应变HER的进一步研究表明，双轴应变可以有效地修饰ΔGHER的H *，可归因于非对称表面拓扑和电荷极化。这些结果不仅提供了合成具有各种表面功能化的碳氮化物MXene的策略，而且提供了通过化学掺杂和应变工程设计的可行解决方案。
更新日期：2021-03-04
中文翻译：
二维碳氮化物MXenes作为氢析出的高效电催化剂
由于其优异的热稳定性，优异的电导率和可调节的表面化学性质，二维过渡金属碳化物，氮化物和碳氮化物（MXenes）非常适合作为氢释放反应（HER）的潜在电催化剂。然而，尽管已经合成了近30种MXene，但到目前为止，实验上报道的碳氮化物MXene较少，但是人们非常希望其潜在的有前途的电化学性能。在这里，我们探讨了Mo 2（CN）T x的热力学有利构型（T = F，OH和O）在各种电化学环境下带有官能团的混合物。结果表明，O * / OH *端基的Mo基碳氮化物MXenes在环境条件下表现出最稳定的状态。通过探索HER在不同的C和N原子比下对各种Mo 2（C x N 1– x）T 2的催化性能，我们发现三个最佳的C / N比为0.5 ML O *和0.5 ML OH * HER的催化活性好于Pt金属。对共官能化的Mo 2（C x N 1– x）OOH的可应变HER的进一步研究表明，双轴应变可以有效地修饰ΔGHER的H *，可归因于非对称表面拓扑和电荷极化。这些结果不仅提供了合成具有各种表面功能化的碳氮化物MXene的策略，而且提供了通过化学掺杂和应变工程设计的可行解决方案。
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