Optimizing Intermediate Adsorption via Heteroatom Ensemble Effect over RuFe Bimetallic Alloy for Enhanced Nitrate Electroreduction to Ammonia DOI
Xinying Zhao, Yuzhuo Jiang, Mengfan Wang

et al.

Advanced Energy Materials, Journal Year: 2023, Volume and Issue: 13(31)

Published: June 30, 2023

Abstract The electrochemical nitrate reduction reaction (NO 3 RR) is a promising approach for removal and NH synthesis at ambient conditions. As complex eight‐electron/nine‐proton transfer process, its performance relies heavily on the adsorption ability of intermediates catalyst surface, which determined by geometric electronic configurations active sites. In this work, heteroatom ensemble effect deliberately triggered over RuFe bimetallic alloy to optimize intermediate NO RR. A record‐high yield rate 118.8 mg h −1 high Faradaic efficiency 92.2% are achieved −1.4 V vs reversible hydrogen electrode, ranking top state‐of‐the‐art. Experimental computational results reveal that characteristics induced play crucial roles. Both Ru Fe display continuous state throughout Fermi level, suggesting electron density benefits whole result, facilitated − , efficient stabilization key intermediates, as well timely desorption simultaneously achieved, thus significantly promoting direct .

Language: Английский

Active hydrogen boosts electrochemical nitrate reduction to ammonia DOI Creative Commons

Kui Fan,

Wenfu Xie, Jinze Li

et al.

Nature Communications, Journal Year: 2022, Volume and Issue: 13(1)

Published: Dec. 27, 2022

Electrochemical nitrate reduction to ammonia is a promising alternative strategy the traditional Haber-Bosch process but suffers from low Faradaic efficiency and limited yield due sluggish multi-electron/proton-involved steps. Herein, we report typical hollow cobalt phosphide nanosphere electrocatalyst assembled on self-supported carbon nanosheet array synthesized with confinement that exhibits an extremely high rate of 8.47 mmol h

Language: Английский

Citations

419

Ampere-level current density ammonia electrochemical synthesis using CuCo nanosheets simulating nitrite reductase bifunctional nature DOI Creative Commons

Jia-Yi Fang,

Qizheng Zheng, Yao‐Yin Lou

et al.

Nature Communications, Journal Year: 2022, Volume and Issue: 13(1)

Published: Dec. 22, 2022

Abstract The development of electrocatalysts capable efficient reduction nitrate (NO 3 − ) to ammonia (NH is drawing increasing interest for the sake low carbon emission and environmental protection. Herein, we present a CuCo bimetallic catalyst able imitate bifunctional nature copper-type nitrite reductase, which could easily remove NO 2 via collaboration two active centers. Indeed, Co acts as an electron/proton donating center, while Cu facilitates x adsorption/association. bio-inspired nanosheet electrocatalyst delivers 100 ± 1% Faradaic efficiency at ampere-level current density 1035 mA cm −2 −0.2 V vs . Reversible Hydrogen Electrode. NH production rate reaches high activity 4.8 mmol h −1 (960 g cat ). A mechanistic study, using electrochemical in situ Fourier transform infrared spectroscopy shell-isolated nanoparticle enhanced Raman spectroscopy, reveals strong synergy between Co, with sites promoting hydrogenation adsorbed *H species. well-modulated coverage *NO led simultaneously selectivity yield.

Language: Английский

Citations

404

Recent advances in nanostructured heterogeneous catalysts for N-cycle electrocatalysis DOI Creative Commons
Jie Liang, Qian Liu, Abdulmohsen Ali Alshehri

et al.

Deleted Journal, Journal Year: 2022, Volume and Issue: 1, P. e9120010 - e9120010

Published: May 30, 2022

To restore the natural nitrogen cycle (N-cycle), artificial N-cycle electrocatalysis with flexibility, sustainability, and compatibility can convert intermittent renewable energy (e.g., wind) to harmful or value-added chemicals minimal carbon emissions. The background of such N-cycles, as fixation, ammonia oxidation, nitrate reduction, is briefly introduced here. discussion emerging nanostructures in various conversion reactions focused on architecture/compositional design, electrochemical performances, reaction mechanisms, instructive tests. Energy device advancements for achieving more functions well in situ/operando characterizations toward understanding key steps are also highlighted. Furthermore, some recently proposed less discussed C–N coupling summarized. We classify inorganic sources that each other under an applied voltage into three types, namely, abundant nitrogen, toxic (nitrite), oxides, useful compounds ammonia, hydrazine, hydroxylamine, goal providing critical insights strategies facilitate development our circular economy.

Language: Английский

Citations

349

Fe/Cu diatomic catalysts for electrochemical nitrate reduction to ammonia DOI Creative Commons
Shuo Zhang,

WU Jiang-hua,

Mengting Zheng

et al.

Nature Communications, Journal Year: 2023, Volume and Issue: 14(1)

Published: June 19, 2023

Electrochemical conversion of nitrate to ammonia offers an efficient approach reducing pollutants and a potential technology for low-temperature low-pressure synthesis. However, the process is limited by multiple competing reactions NO3- adsorption on cathode surfaces. Here, we report Fe/Cu diatomic catalyst holey nitrogen-doped graphene which exhibits high catalytic activities selectivity production. The enables maximum Faradaic efficiency 92.51% (-0.3 V(RHE)) NH3 yield rate 1.08 mmol h-1 mg-1 (at - 0.5 V(RHE)). Computational theoretical analysis reveals that relatively strong interaction between promotes discharge anions. Nitrogen-oxygen bonds are also shown be weakened due existence hetero-atomic dual sites lowers overall reaction barriers. dual-site hetero-atom strategy in this work provides flexible design further development expands electrocatalytic techniques reduction

Language: Английский

Citations

322

Advances in ammonia electrosynthesis from ambient nitrate/nitrite reduction DOI Creative Commons
Jie Liang, Zixiao Li, Longcheng Zhang

et al.

Chem, Journal Year: 2023, Volume and Issue: 9(7), P. 1768 - 1827

Published: June 21, 2023

Language: Английский

Citations

270

Electrochemical Nitrate Reduction: Ammonia Synthesis and the Beyond DOI
Yuecheng Xiong, Yunhao Wang, Jingwen Zhou

et al.

Advanced Materials, Journal Year: 2023, Volume and Issue: 36(17)

Published: June 9, 2023

Natural nitrogen cycle has been severely disrupted by anthropogenic activities. The overuse of N-containing fertilizers induces the increase nitrate level in surface and ground waters, substantial emission oxides causes heavy air pollution. Nitrogen gas, as main component air, used for mass ammonia production over a century, providing enough nutrition agriculture to support world population increase. In last decade, researchers have made great efforts develop processes under ambient conditions combat intensive energy consumption high carbon associated with Haber-Bosch process. Among different techniques, electrochemical reduction reaction (NO

Language: Английский

Citations

214

Electrocatalytic nitrate reduction to ammonia on defective Au1Cu (111) single-atom alloys DOI
Yuanzheng Zhang, Xiang Chen, Weilai Wang

et al.

Applied Catalysis B Environment and Energy, Journal Year: 2022, Volume and Issue: 310, P. 121346 - 121346

Published: March 26, 2022

Language: Английский

Citations

209

Electrocatalytic conversion of nitrate waste into ammonia: a review DOI
Jayaraman Theerthagiri,

Juhyeon Park,

Himadri Tanaya Das

et al.

Environmental Chemistry Letters, Journal Year: 2022, Volume and Issue: 20(5), P. 2929 - 2949

Published: July 9, 2022

Language: Английский

Citations

192

Recent advances in electrocatalytic ammonia synthesis DOI
Ling Ouyang, Jie Liang,

Yongsong Luo

et al.

CHINESE JOURNAL OF CATALYSIS (CHINESE VERSION), Journal Year: 2023, Volume and Issue: 50, P. 6 - 44

Published: July 1, 2023

Language: Английский

Citations

184

Regulating active hydrogen adsorbed on grain boundary defects of nano-nickel for boosting ammonia electrosynthesis from nitrate DOI
Jian Zhou, Ming Wen, Rong Huang

et al.

Energy & Environmental Science, Journal Year: 2023, Volume and Issue: 16(6), P. 2611 - 2620

Published: Jan. 1, 2023

The grain boundary defect engineered Ni nanoparticles has been explored for boosting selective nitrate electroreduction to ammonia, and its NH 3 generation rate is much higher than those of the reported copper or noble metal-based catalysts.

Language: Английский

Citations

178