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Noble-Metal-Metalloid Alloy Architectures: Mesoporous Amorphous Iridium-Tellurium Alloy for Electrochemical N 2 Reduction.

Bo JiangHairong XuePei WangHaoran DuYunqing KangJingjing ZhaoShengyao WangWei ZhouZhenfeng BianHexing LiJoel HenzieYamauchi Yusuke
Published in: Journal of the American Chemical Society (2023)
Amorphous noble metals with high surface areas have attracted significant interest as heterogeneous catalysts due to the numerous dangling bonds and abundant unsaturated surface atoms created by the amorphous phase. However, synthesizing amorphous noble metals with high surface areas remains a significant challenge due to strong isotropic metallic bonds. This paper describes the first example of a mesoporous amorphous noble metal alloy [iridium-tellurium (IrTe)] obtained using a micelle-directed synthesis method. The resulting mesoporous amorphous IrTe electrocatalyst exhibits excellent performance in the electrochemical N 2 reduction reaction. The ammonia yield rate is 34.6 μg mg -1 h -1 with a Faradaic efficiency of 11.2% at -0.15 V versus reversible hydrogen electrode in 0.1 M HCl solution, outperforming comparable crystalline and Ir metal counterparts. The interconnected porous scaffold and amorphous nature of the alloy create a complementary effect that simultaneously enhances N 2 absorption and suppresses the hydrogen evolution reaction. According to theoretical simulations, incorporating Te in the IrTe alloy effectively strengthens the adsorption of N 2 and lowers the Gibbs free energy for the rate-limiting step of the electrocatalytic N 2 reduction reaction. Mesoporous chemistry enables a new route to achieve high-performance amorphous metalloid alloys with properties that facilitate the selective electrocatalytic reduction of N 2 .
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