Nitrogen Fixation via Splitting into Nitrido Complexes DOI
Sebastian J. K. Forrest,

Bastian Schluschaß,

Ekaterina Yu. Yuzik-Klimova

et al.

Chemical Reviews, Journal Year: 2021, Volume and Issue: 121(11), P. 6522 - 6587

Published: May 11, 2021

The large carbon footprint of the Haber–Bosch process, which provides ammonia for fertilizers but also feedstock all nitrogenous commercial products, has fueled quest alternative synthetic strategies to nitrogen fixation. Owing extraordinarily strong N≡N triple bond, key step reaction, i.e., dissociative adsorption N2, requires high temperatures. Since first report in 1995, a wide variety molecular transition metal and f-block compounds have been reported that can fully cleave N2 at ambient conditions form well-defined nitrido complexes. We here provide comprehensive survey current state splitting reactions solution follow-up transfer reactivity. Particular emphasis is put on electronic structure requirements formation suitable precursors their N–N scission prospects synthesis containing products will be discussed, ranging from heterocumulenes organic amines, amides or nitriles via proton coupled electron transfer, carbonylation, electrophilic functionalization derived Accomplishments challenges fixation are presented offer guidelines development catalytic platforms.

Language: Английский

Electrocatalytic reduction of nitrate – a step towards a sustainable nitrogen cycle DOI
Hui Xu, Yuanyuan Ma, Jun Chen

et al.

Chemical Society Reviews, Journal Year: 2022, Volume and Issue: 51(7), P. 2710 - 2758

Published: Jan. 1, 2022

This review provides an overview of electrocatalytic reduction nitrate, including the reaction mechanisms, reactor design principles, product detection methods, and performance evaluation which can provide a sustainable nitrogen cycle.

Language: Английский

Citations

627
Electrocatalytic Refinery for Sustainable Production of Fuels and Chemicals DOI Creative Commons
Cheng Tang, Yao Zheng, Mietek Jaroniec

et al.

Angewandte Chemie International Edition, Journal Year: 2021, Volume and Issue: 60(36), P. 19572 - 19590

Published: Feb. 19, 2021

Abstract Compared to modern fossil‐fuel‐based refineries, the emerging electrocatalytic refinery (e‐refinery) is a more sustainable and environmentally benign strategy convert renewable feedstocks energy sources into transportable fuels value‐added chemicals. A crucial step in conducting e‐refinery processes development of appropriate reactions optimal electrocatalysts for efficient cleavage formation chemical bonds. However, compared well‐studied primary (e.g., O 2 reduction, water splitting), mechanistic aspects materials design complex are yet be settled. To address this challenge, herein, we first present fundamentals heterogeneous electrocatalysis some reactions, then implement these establish framework by coupling situ generated intermediates (integrated reactions) or products (tandem reactions). We also set principles strategies efficiently manipulate reaction pathways.

Language: Английский

Citations

516
Strategies to suppress hydrogen evolution for highly selective electrocatalytic nitrogen reduction: challenges and perspectives DOI
Yongwen Ren,

Chang Yu,

Xinyi Tan

et al.

Energy & Environmental Science, Journal Year: 2021, Volume and Issue: 14(3), P. 1176 - 1193

Published: Jan. 1, 2021

This review underlines the strategies to suppress HER for selective NRR in view of proton-/electron-transfer kinetics, thermodynamics, and electrocatalyst design on basis deep understanding mechanisms.

Language: Английский

Citations

422
The Progress and Outlook of Metal Single-Atom-Site Catalysis DOI
Liang Xiao, Ninghua Fu,

Shuangchao Yao

et al.

Journal of the American Chemical Society, Journal Year: 2022, Volume and Issue: 144(40), P. 18155 - 18174

Published: Sept. 29, 2022

Single-atom-site catalysts (SASCs) featuring maximized atom utilization and isolated active sites have progressed tremendously in recent years as a highly prosperous branch of catalysis research. Varieties SASCs been developed that show excellent performance many catalytic applications. The major goal SASC research is to establish feasible synthetic strategies for the preparation high-performance catalysts, achieve an in-depth understanding active-site structures mechanisms, develop practical with industrial value. This Perspective describes up-to-date development related such dual-atom-site (DASCs) nano-single-atom-site (NSASCs), analyzes current challenges encountered by these applications, proposes their possible future path.

Language: Английский

Citations

376
Comprehensive Understanding of the Thriving Ambient Electrochemical Nitrogen Reduction Reaction DOI
Xue Zhao, Guangzhi Hu, Gao‐Feng Chen

et al.

Advanced Materials, Journal Year: 2021, Volume and Issue: 33(33)

Published: July 1, 2021

Abstract The electrochemical method of combining N 2 and H O to produce ammonia (i.e., the nitrogen reduction reaction [E‐NRR]) continues draw attention as it is both environmentally friendly well suited for a progressively distributed farm economy. Despite multitude recent works on E‐NRR, further progress in this field faces bottleneck. On one hand, despite extensive exploration trial‐and‐error evaluation E‐NRR catalysts, no study has stood out become stage protagonist. other current level production (microgram‐scale) an almost insurmountable obstacle its qualitative quantitative determination, hindering discrimination between true activity contamination. Herein i) popular theory mechanism NRR are introduced; ii) comprehensive summary related catalysts provided; iii) operational procedures addressed, including acquisition key metrics, challenges faced, most suitable solutions; iv) guiding principles standardized recommendations emphasized future research directions prospects provided.

Language: Английский

Citations

372
Pd doping-weakened intermediate adsorption to promote electrocatalytic nitrate reduction on TiO2 nanoarrays for ammonia production and energy supply with zinc–nitrate batteries DOI
Ying Guo, Rong Zhang, Shaoce Zhang

et al.

Energy & Environmental Science, Journal Year: 2021, Volume and Issue: 14(7), P. 3938 - 3944

Published: Jan. 1, 2021

An electrochemical nitrate-based cell enables both ammonia production and energy supply.

Language: Английский

Citations

349
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
Electrochemical oxidation of biomass derived 5-hydroxymethylfurfural (HMF): pathway, mechanism, catalysts and coupling reactions DOI

Yuechao Yang,

Tiancheng Mu

Green Chemistry, Journal Year: 2021, Volume and Issue: 23(12), P. 4228 - 4254

Published: Jan. 1, 2021

HMF electrooxidation is emerging as a powerful and promising method to produce wide range of high-value chemicals on account mild operation conditions, controllable selectivity, scalability.

Language: Английский

Citations

339
Continuous-flow electrosynthesis of ammonia by nitrogen reduction and hydrogen oxidation DOI
Xianbiao Fu, Jakob B. Pedersen, Yuanyuan Zhou

et al.

Science, Journal Year: 2023, Volume and Issue: 379(6633), P. 707 - 712

Published: Feb. 16, 2023

Ammonia is a critical component in fertilizers, pharmaceuticals, and fine chemicals an ideal, carbon-free fuel. Recently, lithium-mediated nitrogen reduction has proven to be promising route for electrochemical ammonia synthesis at ambient conditions. In this work, we report continuous-flow electrolyzer equipped with 25-square centimeter-effective area gas diffusion electrodes wherein coupled hydrogen oxidation. We show that the classical catalyst platinum not stable oxidation organic electrolyte, but platinum-gold alloy lowers anode potential avoids decremental decomposition of electrolyte. At optimal operating conditions, achieve, 1 bar, faradaic efficiency production up 61 ± 1% energy 13 current density -6 milliamperes per square centimeter.

Language: Английский

Citations

313
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

293