电化学 CO2 还原过程中氧化物衍生的 PdIn 纳米催化剂的电位和时间相关动态特性,ACS Nano

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电化学 CO2 还原过程中氧化物衍生的 PdIn 纳米催化剂的电位和时间相关动态特性
ACS Nano ( IF 15.8 ) Pub Date : 2022-04-04 , DOI: 10.1021/acsnano.1c11664
Debabrata Bagchi _{1,

2} , Shreya Sarkar _{1,

2} , Ashutosh Kumar Singh _{2,

3} , Chathakudath P Vinod ₄ , Sebastian C Peter _{1,

2}

Affiliation

_{将 CO 2}电化学还原为有价值的燃料和化学品是通过减少 CO ₂排放和最小化其对气候的不利影响来替代化石燃料的有前途的途径。已经进行了巨大的努力来设计有效的催化剂材料以通过电化学过程从CO ₂中以高产率选择性地生产所需的产物。在这项工作中，报告了一种通过在金属基合金 (PdIn) 纳米颗粒和氧化物₍_In₂ O ₃), 这是通过简单的溶液法合成的。氧化物衍生的 PdIn 表面显示出出色的 eCO ₂ RR 活性和增强的 CO 选择性，法拉第效率 (FE) 在 -0.9 V（相对于 RHE）时为 92.13%。另一方面，由于裸 PdIn 合金上的电荷转移而导致的表面 PdO 形成降低了 CO ₂ RR 活性。在原位（EXAFS 和 IR）和非原位（XPS、拉曼）光谱技术的支持下，Pd-In-O 界面的最佳存在已被确定为增强 eCO ₂ RR 对 CO 还原反应的关键参数气氛。据报道，eCO ₂ RR 持续时间的影响通过将产品选择性从 H _{2切换为影响整体性能}（来自水还原）到氧化物衍生合金表面上的CO（来自 eCO _{2 RR）。}这项工作还通过使用气体扩散电极 (GDE) 并在流通池配置中优化其工艺参数，成功地成倍提高了电流密度。

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Potential- and Time-Dependent Dynamic Nature of an Oxide-Derived PdIn Nanocatalyst during Electrochemical CO2 Reduction

Electrochemical reduction of CO₂ into valuable fuels and chemicals is a promising route of replacing fossil fuels by reducing CO₂ emissions and minimizing its adverse effects on the climate. Tremendous efforts have been carried out for designing efficient catalyst materials to selectively produce the desired product in high yield from CO₂ by the electrochemical process. In this work, a strategy is reported to enhance the electrochemical CO₂ reduction reaction (ECO₂RR) by constructing an interface between a metal-based alloy (PdIn) nanoparticle and an oxide (In₂O₃), which was synthesized by a facile solution method. The oxide-derived PdIn surface has shown excellent eCO₂RR activity and enhanced CO selectivity with a Faradaic efficiency (FE) of 92.13% at −0.9 V (vs RHE). On the other hand, surface PdO formation due to charge transfer on the bare PdIn alloy reduces the CO₂RR activity. With the support of in situ (EXAFS and IR) and ex situ (XPS, Raman) spectroscopic techniques, the optimum presence of the Pd–In–O interface has been identified as a crucial parameter for enhancing eCO₂RR toward CO in a reducing atmosphere. The influence of eCO₂RR duration is reported to affect the overall performance by switching the product selectivity from H₂ (from water reduction) to CO (from eCO₂RR) on the oxide-derived alloy surface. This work also succeeded in the multifold enhancement of the current density by employing the gas diffusion electrode (GDE) and optimizing its process parameters in a flow cell configuration.

更新日期：2022-04-04

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