Soumita Chakraborty, Daizy Kalita, Sakshi Agarwal, Surishi Vashishth, Nijita Mathew, Sisir Maity, Devender Goud, Ankit Rao, Sebastian C. Peter, Abhishek K. Singh and Muthusamy Eswaramoorthy*,
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引用次数: 0
摘要
电化学制取 H2 和减少 CO2 可解决困扰全球的能源和环境危机。高效的电催化剂要求这些反应具有最低的过电位。鉴于钯在火山图上的位置接近铂,因此钯是氢进化反应(HER)的可行替代品。不过,其活性受到高过电位的限制。由于 d 带中心的有利位置,钯还是二氧化碳还原反应(CO2RR)的良好电催化剂。然而,活性位点的 CO 中毒导致电催化稳定性较低。在此,我们报告了一种掺入镍的钯催化剂 NiPd,它能在 25 mV (η10) 的超低过电位下将水还原成 H2。此外,它还能在 -0.25 V 的电位(相对于 RHE)下将 CO2 还原成甲酸盐,远化效率高达 97%。DFT 研究表明,由于催化剂表面的弯曲吸附构型,镍的加入使 CO2 易于活化。经反应后表征研究证明,NiPd 催化剂在 HER(400 小时)和 CO2RR(9 小时)中表现出强大而稳定的性能,并具有较高的结构完整性。
Tuning the Electrocatalytic Activity of Pd Nanocatalyst toward Hydrogen Evolution and Carbon Dioxide Reduction Reactions by Nickel Incorporation
Electrochemical H2 generation and CO2 reduction address the energy and environmental crisis plaguing the world. An efficient electrocatalyst would require the lowest overpotential for these reactions. Given its position on the volcano plot near platinum, palladium presents itself as a viable alternative for the hydrogen evolution reaction (HER). However, the activity is limited by a high overpotential. It is also a good electrocatalyst for the CO2 reduction reaction (CO2RR) due to the favorable position of the d-band center. Nevertheless, the CO poisoning of the active site results in low electrocatalytic stability. Herein, we report a Ni-incorporated palladium catalyst, NiPd, which reduces water to H2 at a very low overpotential of 25 mV (η10). Furthermore, it reduces CO2 to formate with a very high faradaic efficiency of 97% at a potential of −0.25 V (vs RHE). DFT studies show that Ni inclusion leads to the facile activation of CO2 due to a bent adsorption configuration at the catalyst surface. The NiPd catalyst exhibits a strong and stable performance for HER (400 h) as well as for CO2RR (9 h) with high structural integrity as proven by postreaction characterization studies.
期刊介绍:
The journal Chemistry of Materials focuses on publishing original research at the intersection of materials science and chemistry. The studies published in the journal involve chemistry as a prominent component and explore topics such as the design, synthesis, characterization, processing, understanding, and application of functional or potentially functional materials. The journal covers various areas of interest, including inorganic and organic solid-state chemistry, nanomaterials, biomaterials, thin films and polymers, and composite/hybrid materials. The journal particularly seeks papers that highlight the creation or development of innovative materials with novel optical, electrical, magnetic, catalytic, or mechanical properties. It is essential that manuscripts on these topics have a primary focus on the chemistry of materials and represent a significant advancement compared to prior research. Before external reviews are sought, submitted manuscripts undergo a review process by a minimum of two editors to ensure their appropriateness for the journal and the presence of sufficient evidence of a significant advance that will be of broad interest to the materials chemistry community.