Recent Advances in Electrocatalytic Hydrogenation Reactions on Copper‐Based Catalysts DOI Creative Commons
Min Zheng, Junyu Zhang, Pengtang Wang

et al.

Advanced Materials, Journal Year: 2023, Volume and Issue: 36(14)

Published: Sept. 27, 2023

Hydrogenation reactions play a critical role in the synthesis of value-added products within chemical industry. Electrocatalytic hydrogenation (ECH) using water as hydrogen source has emerged an alternative to conventional thermocatalytic processes for sustainable and decentralized under mild conditions. Among various ECH catalysts, copper-based (Cu-based) nanomaterials are promising candidates due their earth-abundance, unique electronic structure, versatility, high activity/selectivity. Herein, recent advances application Cu-based catalysts upgrading valuable chemicals systematically analyzed. The properties initially introduced, followed by design strategies enhance activity selectivity. Then, typical on presented detail, including carbon dioxide reduction multicarbon generation, alkyne-to-alkene conversion, selective aldehyde ammonia production from nitrogen-containing substances, amine organic nitrogen compounds. In these catalyst composition nanostructures toward different is focused. co-hydrogenation two substrates (e.g., CO

Language: Английский

Tandem Electrocatalytic Nitrate Reduction to Ammonia on MBenes DOI
Guike Zhang, Xiaotian Li, Kai Chen

et al.

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(13)

Published: Feb. 3, 2023

We demonstrate the great feasibility of MBenes as a new class tandem catalysts for electrocatalytic nitrate reduction to ammonia (NO3 RR). As proof concept, FeB2 is first employed model MBene catalyst NO3 RR, showing maximum NH3 -Faradaic efficiency 96.8 % with corresponding yield 25.5 mg h-1 cm-2 at -0.6 V vs. RHE. Mechanistic studies reveal that exceptional RR activity arises from catalysis mechanism, is, B sites activate NO3- form intermediates, while Fe dissociate H2 O and increase *H supply on promote intermediate hydrogenation enhance -to-NH3 conversion.

Language: Английский

Citations

295

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

281

Single‐Atom Bi Alloyed Pd Metallene for Nitrate Electroreduction to Ammonia DOI
Kai Chen,

Ziyu Ma,

Xingchuan Li

et al.

Advanced Functional Materials, Journal Year: 2023, Volume and Issue: 33(12)

Published: Jan. 15, 2023

Abstract Electrochemical reduction of nitrate to ammonia (NO 3 RR) holds a great promise for attaining both NH electrosynthesis and wastewater purification. Herein, single‐atom Bi alloyed Pd metallene (Bi 1 Pd) is reported as highly effective NO RR catalyst, showing near 100% ‐Faradaic efficiency with the corresponding yield 33.8 mg h −1 cm −2 at −0.6 V versus RHE, surpassing those almost all ever catalysts. In‐depth theoretical operando spectroscopic investigations unveil that electronically couples its neighboring atoms synergistically activate − destabilize *NO on Pd, leading reduced energy barrier potential‐determining step (*NO→*NOH) enhanced protonation energetics ‐to‐NH pathway.

Language: Английский

Citations

234

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

232

Defect engineering of two-dimensional materials for advanced energy conversion and storage DOI
Fu Liu, Zhanxi Fan

Chemical Society Reviews, Journal Year: 2023, Volume and Issue: 52(5), P. 1723 - 1772

Published: Jan. 1, 2023

Defective two-dimensional (2D) materials show huge potential for energy-related fields. This review overviews the formation/evolution mechanisms and engineering strategies of defects in 2D materials, which enable enhanced electrode reaction kinetics.

Language: Английский

Citations

211

Microenvironment Engineering of Single/Dual‐Atom Catalysts for Electrocatalytic Application DOI Open Access
Yun Gao, Baozhong Liu, Dingsheng Wang

et al.

Advanced Materials, Journal Year: 2023, Volume and Issue: 35(31)

Published: Feb. 23, 2023

Single/dual-metal atoms supported on carbon matrix can be modulated by coordination structure and neighboring active sites. Precisely designing the geometric electronic uncovering structure-property relationships of single/dual-metal confront with grand challenges. Herein, this review summarizes latest progress in microenvironment engineering single/dual-atom sites via a comprehensive comparison single-atom catalyst (SACs) dual-atom catalysts (DACs) term design principles, modulation strategy, theoretical understanding structure-performance correlations. Subsequently, recent advances several typical electrocatalysis process are discussed to get general reaction mechanisms finely-tuned SACs DACs. Finally, full-scaled summaries challenges prospects given for This will provide new inspiration development atomically dispersed electrocatalytic application.

Language: Английский

Citations

187

Breaking Local Charge Symmetry of Iron Single Atoms for Efficient Electrocatalytic Nitrate Reduction to Ammonia DOI
Jingwen Xu,

Shengbo Zhang,

Hengjie Liu

et al.

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(39)

Published: July 22, 2023

The electrochemical conversion of nitrate pollutants into value-added ammonia is a feasible way to achieve artificial nitrogen cycle. However, the development electrocatalytic nitrate-to-ammonia reduction reaction (NO3- RR) has been hampered by high overpotential and low Faradaic efficiency. Here we develop an iron single-atom catalyst coordinated with phosphorus on hollow carbon polyhedron (denoted as Fe-N/P-C) NO3- RR electrocatalyst. Owing tuning effect atoms breaking local charge symmetry single-Fe-atom catalyst, it facilitates adsorption ions enrichment some key intermediates during process. Fe-N/P-C exhibits 90.3 % efficiency yield rate 17980 μg h-1 mgcat-1 , greatly outperforming reported Fe-based catalysts. Furthermore, operando SR-FTIR spectroscopy measurements reveal pathway based observed under different applied potentials durations. Density functional theory calculations demonstrate that optimized free energy ascribed asymmetric atomic interface configuration, which achieves optimal electron density distribution. This work demonstrates critical role atomic-level precision modulation heteroatom doping for RR, providing effective strategy improving catalytic performance single atom catalysts in reactions.

Language: Английский

Citations

166

Electrocatalytic Hydrogenation Boosts Reduction of Nitrate to Ammonia over Single-Atom Cu with Cu(I)-N3C1 Sites DOI
Yinghao Xue,

Qihui Yu,

Ma Qian

et al.

Environmental Science & Technology, Journal Year: 2022, Volume and Issue: 56(20), P. 14797 - 14807

Published: Sept. 29, 2022

The conversion of nitrate to ammonia can serve two important functions: mitigating pollution and offering a low energy intensity pathway for synthesis. Conventional synthesis from electrocatalytic reduction reactions (NO3RR) is often impeded by incomplete conversion, sluggish kinetics, the competition hydrogen evolution reactions. Herein, atomic Cu sites anchored on micro-/mesoporous nitrogen-doped carbon (Cu MNC) with fine-tuned hydrophilicity, channels, abundant Cu(I) were synthesized selective ammonia, achieving ambient temperature pressure hydrogenation nitrate. Laboratory experiments demonstrated that catalyst has an yield rate per active site 5466 mmol gCu-1 h-1 transformed 94.8% in wastewater containing 100 mg-N L-1 near drinking water standard (MCL 5 L-1) at -0.64 V vs RHE. Extended X-ray absorption fine structure (EXAFS) theoretical calculations showed coordination environment (Cu(I)-N3C1) localizes charge around central atoms adsorbs *NO3 *H onto neighboring C balanced adsorption energy. Cu(I)-N3C1 moieties reduce activation rate-limiting steps (*HNO3 → *NO2, *NH2 *NH3) compared conventional Cu(II)-N4 lead thermodynamically favorable process NH3. as-prepared cell run continuously 84 h (14 cycles) produce 21.7 mgNH3 only 5.64 × 10-3 kWh consumption, suitable decentralized removal nitrate-containing wastewater.

Language: Английский

Citations

162

Recent Advances in Electrocatalysts for Efficient Nitrate Reduction to Ammonia DOI
Di Liu, Lulu Qiao,

Shuyang Peng

et al.

Advanced Functional Materials, Journal Year: 2023, Volume and Issue: 33(43)

Published: June 25, 2023

Abstract Ammonia as an irreplaceable chemical has been widely demanded to keep the sustainable development of modern society. However, its industrial production consumes huge energy and releases extraordinary green‐house gases, leading various environmental issues. To achieve green ammonia is a great challenge that extensively pursued recently. In review, most promising strategy, electrochemical nitrate reduction reaction (e‐NO 3 RR) for purpose comprehensively investigated give full understanding mechanism provide guidance future directions. Particularly, electrocatalysts focused realize high yield rate Faraday efficiency applications. The recent‐developed catalysts, including noble metallic materials, alloys, metal compounds, single‐metal‐atom metal‐free are systematically discussed review effects factors on catalytic performance in e‐NO RR. Accordingly, strategies, defects engineering, coordination environment modulating, surface controlling, hybridization, carefully improve performance, such intrinsic activity selectivity. Finally, perspectives challenges given out. This shall insightful advanced systems efficiently industry.

Language: Английский

Citations

150

Recent progress and strategies on the design of catalysts for electrochemical ammonia synthesis from nitrate reduction DOI
Wei Song,

Luchao Yue,

Xiaoya Fan

et al.

Inorganic Chemistry Frontiers, Journal Year: 2023, Volume and Issue: 10(12), P. 3489 - 3514

Published: Jan. 1, 2023

Ammonia (NH3) is an essential raw material in the production of fertilizers and a promising carbon-free energy carrier, however, its synthesis still depends on energy- capital-intensive Haber–Bosch process. Recently, electrochemical N2 reduction reaction has attracted significant interest as emerging method for NH3 under ambient conditions. However, limited solubility aqueous electrolyte strong NN bonds result low yield rate, inferior faradaic efficiency unsatisfactory selectivity, impeding further practical application. Considering high water nitrate (NO3−), NO3− (NO3−RR) become fascinating route achieving sustainable NH3, enormous progress been made this field. As consequence, review discusses mechanism systematically summarizes recent development electrocatalysts NO3−RR, including noble-metal-based materials, single-atom metal catalysts, transition-metal-based catalysts. Diverse design strategies catalysts to boost NO3−RR performance, such defect engineering, rational structure design, strain engineering constructing heterostructures, are discussed. This followed by illustration how robust understanding optimization affords fundamental insights into efficiency, selectivity electrocatalysts. Finally, we conclude with future perspectives critical issues, challenges research directions high-efficiency selective NH3.

Language: Английский

Citations

125