无定形固体
介孔材料
贵金属
化学
电催化剂
合金
化学工程
铱
电化学
非晶态金属
材料科学
无机化学
催化作用
金属
电极
物理化学
结晶学
有机化学
工程类
作者
Bo Jiang,Hairong Xue,Pei Wang,Haoran Du,Yunqing Kang,Jingjing Zhao,Shengyao Wang,Wei Zhou,Zhenfeng Bian,Hexing Li,Joel Henzie,Yusuke Yamauchi
摘要
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 N2 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 N2 absorption and suppresses the hydrogen evolution reaction. According to theoretical simulations, incorporating Te in the IrTe alloy effectively strengthens the adsorption of N2 and lowers the Gibbs free energy for the rate-limiting step of the electrocatalytic N2 reduction reaction. Mesoporous chemistry enables a new route to achieve high-performance amorphous metalloid alloys with properties that facilitate the selective electrocatalytic reduction of N2.
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