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Interface-induced enhancement of paired electrolysis in 5-hydroxymethylfurfural-H2O system on symbiotic nickel/molybdenum nitride heterostructure
Chemical Engineering Journal ( IF 13.3 ) Pub Date : 2023-10-07 , DOI: 10.1016/j.cej.2023.146490
Siyu Ma , Zhihao Wang , Bowen Liu , Xiaolei Wang , Shichao Du , Zichen Song , Xinxin Bian , Manchen Hao , Ju Huang , Zhimin Chen , Zhiyu Ren

Pairing the hydrogen evolution reaction (HER) with the thermodynamics-friendly electrooxidation reaction (EOR) is a powerful way to maximize the energy/economic effectiveness, but still a challenge. Herein, the symbiotic Ni/MoN heterojunction arrays were constructed on foam (Ni/MoN/NF) by the nitridation-induced in situ reduction/conversion strategy. The fascinating interfacial electronic structure and surface reconstruction of Ni/MoN/NF heterojunction are responsible for the enhanced HMF-H2O paired electrolysis. Ni/MoN/NF only requires a low overpotential of 53 mV to reach the HER current density of 10 mA cm−2, as well as the good durability; and NiOOH derived on the anode are electronically activated by MoN to achieving high-efficiency conversion from HMF to FDCA (∼100 % conversion, 97.5 % yield and 97.4 % Faradaic efficiency). For the HMF-H2O paired electrolysis, the assembled Ni/MoN/NF||Ni/MoN/NF electrolyzer only requires a low potential of 1.391 V to yield the current density of 10 mA cm−2, ranking at the forefront in the reported coupling catalysts. Theoretical calculations manifest that the upshift of d-band center of the NiOOH/MoN heterojunction contributes to HMF chemisorption and activation, thereby enhancing its catalytic activity towards HMFEOR. Our study sheds light on the significance of designing the paired electrolysis with low voltage input for renewable energy applications.



中文翻译:

共生镍/氮化钼异质结构上 5-羟甲基糠醛-H2O 体系中界面诱导增强配对电解

将析氢反应 (HER) 与热力学友好的电氧化反应 (EOR) 结合起来是最大限度提高能源/经济效益的有效方法,但仍然是一个挑战。在此,通过氮化诱导的原位还原/转化策略在泡沫(Ni/MoN/NF)上构建了共生Ni/MoN异质结阵列。Ni/MoN/NF异质结迷人的界面电子结构和表面重构是增强HMF-H 2 O配对电解的原因。Ni/MoN/NF仅需53 mV的低过电位即可达到10 mA cm -2的HER电流密度,并且具有良好的耐久性;阳极上衍生的 NiOOH 被 MoN 电子激活,实现从 HMF 到 FDCA 的高效转化(~100% 转化率、97.5% 产率和 97.4% 法拉第效率)。对于HMF-H 2 O配对电解,组装的Ni/MoN/NF||Ni/MoN/NF电解槽仅需1.391 V的低电势即可产生10 mA cm -2 的电流密度,在同类电解中排名前列。报道的偶联催化剂。理论计算表明,NiOOH/MoN异质结d带中心的上移有助于HMF的化学吸附和活化,从而增强其对HMFEOR的催化活性。我们的研究揭示了为可再生能源应用设计低电压输入配对电解的重要性。

更新日期:2023-10-07
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