TY - JOUR
T1 - Highly Stable Perovskite Oxides for Electrocatalytic Acidic NOx− Reduction Streamlining Ammonia Synthesis from Air
AU - Guo, Xuecheng
AU - Wang, Zhongliao
AU - Gao, Yuan
AU - Zhang, Chao
AU - Zhang, Shuai
AU - Sang, Shuaikang
AU - Ma, Jun
AU - Sun, Shuhui
AU - Murzin, Dmitry Yu
AU - Low, Jingxiang
AU - Shao, Tao
AU - Xiong, Yujie
N1 - Publisher Copyright:
© 2024 Wiley-VCH GmbH.
PY - 2024/10/1
Y1 - 2024/10/1
N2 - Electrochemical nitrogen oxide ions reduction reaction (NOx−RR) shows great opportunity for ammonia production under ambient conditions. Yet, performing NOx−RR in strong acidic conditions remains challenging due to the corrosion effect on the catalyst and competing hydrogen evolution reactions. Here, we demonstrate a stable La1.5Sr0.5Ni0.5Fe0.5O4 perovskite oxide for the NOx−RR at pH 0, achieving a Faradaic efficiency for ammonia of approaching 100 % at a current density of 2 A cm−2 in a H-type cell. At industrially relevant current density, the NOx−RR system shows stable cell voltage and Faradaic efficiency for >350 h in membrane electrode assembly (MEA) at pH 0. By integrating the catalyst in a stacked MEA with a series connection, we have successfully obtained a record-breaking 2.578 g h−1 NH3 production rate at 20 A. This catalyst‘s unique acid-operability streamlines downstream ammonia utilization for direct ammonium salt production and upstream integration with NOx sources. Techno-economic and lifecycle assessments reveal substantial economic advantages for this ammonia production strategy, even when coupled with a plasma-based NOx production system, presenting a sustainable complement to the conventional Haber–Bosch process.
AB - Electrochemical nitrogen oxide ions reduction reaction (NOx−RR) shows great opportunity for ammonia production under ambient conditions. Yet, performing NOx−RR in strong acidic conditions remains challenging due to the corrosion effect on the catalyst and competing hydrogen evolution reactions. Here, we demonstrate a stable La1.5Sr0.5Ni0.5Fe0.5O4 perovskite oxide for the NOx−RR at pH 0, achieving a Faradaic efficiency for ammonia of approaching 100 % at a current density of 2 A cm−2 in a H-type cell. At industrially relevant current density, the NOx−RR system shows stable cell voltage and Faradaic efficiency for >350 h in membrane electrode assembly (MEA) at pH 0. By integrating the catalyst in a stacked MEA with a series connection, we have successfully obtained a record-breaking 2.578 g h−1 NH3 production rate at 20 A. This catalyst‘s unique acid-operability streamlines downstream ammonia utilization for direct ammonium salt production and upstream integration with NOx sources. Techno-economic and lifecycle assessments reveal substantial economic advantages for this ammonia production strategy, even when coupled with a plasma-based NOx production system, presenting a sustainable complement to the conventional Haber–Bosch process.
KW - economical efficiency
KW - electrocatalytic reduction
KW - NO-to-ammonia
KW - sustainable ammonia production
UR - http://www.scopus.com/inward/record.url?scp=85201061474&partnerID=8YFLogxK
U2 - 10.1002/anie.202410517
DO - 10.1002/anie.202410517
M3 - Article
C2 - 38896017
AN - SCOPUS:85201061474
SN - 1433-7851
VL - 63
JO - Angewandte Chemie International Edition
JF - Angewandte Chemie International Edition
IS - 40
M1 - e202410517
ER -