通过杂原子掺杂策略加速铜晶界位点上工业级 NO3− 电还原为氨,Small

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通过杂原子掺杂策略加速铜晶界位点上工业级 NO3− 电还原为氨
Small ( IF 13.0 ) Pub Date : 2023-05-17 , DOI: 10.1002/smll.202302295
Yan Wang ₁ , Shuai Xia ₁ , Rui Cai ₁ , Jianfang Zhang ₁ , Jiarui Wang ₁ , Cuiping Yu ₁ , Jiewu Cui ₁ , Yong Zhang ₁ , Jingjie Wu ₂ , Shize Yang ₃ , Hark Hoe Tan ₄ , Yucheng Wu _{1,

5,

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Affiliation

尽管电催化硝酸盐还原反应(NO ₃⁻ RR)是一种有吸引力的NH ₃合成路线，但由于缺乏有效的催化剂，其产率较低。在这里，这项工作报告了一种新型的富含晶界（GB）的Sn-Cu催化剂，该催化剂源自Sn掺杂的CuO纳米花的原位电还原，可有效地将NO 3 - 电化学_转化^为NH ₃。优化的Sn _{1% -Cu电极实现了1.98 mmol h}^-1 cm ^-2的高NH ₃产率和-425 mA cm ^-2的工业级电流密度相对于可逆氢电极 (RHE)，在 -0.55 V 时的电压，在 -0.51 V 时相对于 RHE 的最大法拉第效率为 98.2%，优于纯铜电极。原位拉曼和衰减全反射傅里叶变换红外光谱通过监测反应中间体的吸附性质揭示了NO ₃^- RR到NH _{3的反应途径。}密度泛函理论计算表明，高密度GB活性位点和Sn掺杂引起的竞争性析氢反应（HER）抑制协同促进NO ₃^- RR高活性和选择性的NH ₃合成。_{这项工作为高效 NH 3}铺平了道路通过杂原子掺杂原位重建 GB 位点来合成 Cu 催化剂。

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Accelerating Industrial-Level NO3− Electroreduction to Ammonia on Cu Grain Boundary Sites via Heteroatom Doping Strategy

Although the electrocatalytic nitrate reduction reaction (NO₃⁻RR) is an attractive NH₃ synthesis route, it suffers from low yield due to the lack of efficient catalysts. Here, this work reports a novel grain boundary (GB)-rich Sn-Cu catalyst, derived from in situ electroreduction of Sn-doped CuO nanoflower, for effectively electrochemical converting NO₃⁻ to NH₃. The optimized Sn_1%-Cu electrode achieves a high NH₃ yield rate of 1.98 mmol h⁻¹ cm⁻² with an industrial-level current density of −425 mA cm⁻² at −0.55 V versus a reversible hydrogen electrode (RHE) and a maximum Faradaic efficiency of 98.2% at −0.51 V versus RHE, outperforming the pure Cu electrode. In situ Raman and attenuated total reflection Fourier transform infrared spectroscopies reveal the reaction pathway of NO₃⁻RR to NH₃ by monitoring the adsorption property of reaction intermediates. Density functional theory calculations clarify that the high-density GB active sites and the competitive hydrogen evolution reaction (HER) suppression induced by Sn doping synergistically promote highly active and selective NH₃ synthesis from NO₃⁻RR. This work paves an avenue for efficient NH₃ synthesis over Cu catalyst by in situ reconstruction of GB sites with heteroatom doping.

更新日期：2023-05-17

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