Unconventional phase high-entropy nanoalloys with modulated electronic structure for efficient low-concentration nitrate electroreduction to ammonia

10 Aug 2026

Published on nature water (10 August 2026)

Author(s): Fu Liu (刘甫), Fengkun Hao (郝风坤), Mingzi Sun (孙明子), Helin Wang (王鹤林), Ning Yao (姚宁), Yunhao Wang (王云豪), Juan Wang (王娟), Peng Chen (陈鹏), Xintao Ma (马鑫涛), Jingwen Zhou (周静雯), Yuecheng Xiong (熊岳城), Yangbo Ma (马洋博), Guozhi Wang (王国治), Liang Guo (国梁), Xiang Meng (孟翔), Mingzheng Shao (邵明政), Chaohui Wang (王超辉), Miao Wang (王淼), Fangren Qian (钱方仁), Chenliang Ye (叶陈良), Shibo Xi (席识博), Bolong Huang (黄勃龙) & Zhanxi Fan (范战西)

Abstract

Phase control of alloy nanomaterials can modulate their atomic/electronic structures towards various electrocatalytic applications. However, the controlled synthesis of high-entropy nanoalloys (HENAs) with unconventional phase remains challenging. Here we report the one-pot synthesis of RhCuNiInSb HENAs with the unconventional 2H phase through regulating the nucleation/growth kinetics. Compared with the face-centred cubic phase counterpart, 2H RhCuNiInSb HENAs exhibit superior electrocatalytic nitrate reduction performance at low nitrate concentration. Ex/in situ studies reveal the accelerated deoxygenation/hydrogenation kinetics and distinct reaction pathway. Theoretical calculations demonstrate the electronic optimizations induced by the face-centred-cubic-to-2H phase transition, where the electronic redistribution and p–d elemental interactions improve the surface electroactivity. When operated in flow cell, 0.5 l of simulated wastewater can be efficiently converted into the value-added ammonia-derived product within 10 h. With a 20-h electrolysis, the NO3−-N concentration in real industrial and agricultural wastewater can be both reduced above the World Health Organization standard for drinking water.