材料科学
电化学
纳米棒
电催化剂
X射线光电子能谱
解吸
吸附
化学工程
可逆氢电极
无机化学
纳米技术
物理化学
电极
化学
工作电极
工程类
作者
Juan Wang,Bolong Huang,Yujin Ji,Mingzi Sun,Tong Wu,Rongguan Yin,Xing Zhu,Youyong Li,Qi Shao,Xiaoqing Huang
标识
DOI:10.1002/adma.201907112
摘要
Abstract Electrochemical conversion of nitrogen (N 2 ) into value‐added ammonia (NH 3 ) is highly desirable yet formidably challenging due to the extreme inertness of the N 2 molecule, which makes the development of a robust electrocatalyst prerequisite. Herein, a new class of bullet‐like M‐Te (M = Ru, Rh, Ir) glassy porous nanorods (PNRs) is reported as excellent electrocatalysts for N 2 reduction reaction (NRR). The optimized IrTe 4 PNRs present superior activity with the highest NH 3 yield rate (51.1 µg h −1 mg −1 cat. ) and Faraday efficiency (15.3%), as well as long‐term stability of up to 20 consecutive cycles, making them among the most active NRR electrocatalysts reported to date. Both the N 2 temperature‐programmed desorption and valence band X‐ray photoelectron spectroscopy data show that the strong chemical adsorption of N 2 is the key for enhancing the NRR and suppressing the hydrogen evolution reaction of IrTe 4 PNRs. Density functional theory calculations comprehensively identify that the superior adsorption strength of IrTe 4 adsorptions originates from the synergistic collaboration between electron‐rich Ir and the highly electroactive surrounding Te atoms. The optimal adsorption of both N 2 and H 2 O in alkaline media guarantees the superior consecutive NRR process. This work opens a new avenue for designing high‐performance NRR electrocatalysts based on glassy materials.
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