Architecture Engineering and Phase Engineering of Rhodium Metallene Co‐Boost Nitrite‐to‐Ammonia Electroconversion
Zi‐Han Yuan, Bin Sun, Wei Zhong, Xuan Ai, Jianzhi Gao, Ligang Feng, Yu Chen
Abstract
Abstract Electrocatalytic nitrite reduction reaction (NO 2 RR) offers an effective strategy for sustainable ammonia (NH 3 ) synthesis and N‐pollutants wastewater degradation. Herein, we propose a dual‐engineering strategy by combining architecture engineering and phase engineering on nanosheet‐like rhodium metallene (Rh‐NS) coupled with twisted nanoribbon‐like rhodium metallene (Rh‐NR) nanoarchitectonics (Rh‐NS/Rh‐NR) to boost NO 2 − ‐to‐NH 3 electroconversion. Rh‐NS/Rh‐NR, characterized by a high density of unsaturated coordination sites and a large specific surface area, greatly enhances the adsorption capacity of NO 2 − and crucial intermediates and lowers the energy barrier for the rate‐determining step of *NOH formation from *NO. Consequently, Rh‐NS/Rh‐NR exhibits satisfactory Faradaic efficiency (FE) of 98.7% and a remarkable NH 3 yield rate of 44.3 mg mg cat −1 h −1 for NO 2 RR at high reduction potential (0.00 V). Using Rh‐NS/Rh‐NR as cathode, the assembled zinc–nitrite battery delivers excellent discharge performance (24.2 mW cm −2 ) and promising NH 3 synthesis capacity (5.96 mg mg cat −1 h −1 ). This work not only guides the architecture‐engineering design of metallene but also demonstrates the practical potential of zinc–nitrite batteries in integrated energy‐environmental applications.