• 文献标题:   Direct Synthesis of Ammonia from Nitrate on Amorphous Graphene with Near 100% Efficiency
  • 文献类型:   Article
  • 作  者:   HUANG LB, CHENG L, MA TH, ZHANG JJ, WU HK, SU JJ, SONG Y, ZHU H, LIU Q, ZHU MH, ZENG ZY, HE QY, TSE MK, YANG DT, YAKOBSON BI, TANG BZ, REN Y, YE RQ
  • 作者关键词:   ammonia synthesi, amorphous graphene, laser induction, nitrate reduction, wastewater remediation
  • 出版物名称:   ADVANCED MATERIALS
  • ISSN:   0935-9648 EI 1521-4095
  • 通讯作者地址:  
  • 被引频次:   5
  • DOI:   10.1002/adma.202211856 EA APR 2023
  • 出版年:   2023

▎ 摘  要

Ammonia is an indispensable commodity in the agricultural and pharmaceutical industries. Direct nitrate-to-ammonia electroreduction is a decentralized route yet challenged by competing side reactions. Most catalysts are metal-based, and metal-free catalysts with high nitrate-to-ammonia conversion activity are rarely reported. Herein, it is shown that amorphous graphene synthesized by laser induction and comprising strained and disordered pentagons, hexagons, and heptagons can electrocatalyze the eight-electron reduction of NO3- to NH3 with a Faradaic efficiency of approximate to 100% and an ammonia production rate of 2859 mu g cm(-2) h(-1) at -0.93 V versus reversible hydrogen electrode. X-ray pair-distribution function analysis and electron microscopy reveal the unique molecular features of amorphous graphene that facilitate NO3- reduction. In situ Fourier transform infrared spectroscopy and theoretical calculations establish the critical role of these features in stabilizing the reaction intermediates via structural relaxation. The enhanced catalytic activity enables the implementation of flow electrolysis for the on-demand synthesis and release of ammonia with >70% selectivity, resulting in significantly increased yields and survival rates when applied to plant cultivation. The results of this study show significant promise for remediating nitrate-polluted water and completing the NOx cycle.