High yield electrosynthesis of oxygenates from CO using a relay Cu-Ag co-catalyst system DOI Creative Commons
Nannan Meng, Zhitan Wu, Yanmei Huang

et al.

Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)

Published: May 8, 2024

Abstract As a sustainable alternative to fossil fuel-based manufacture of bulk oxygenates, electrochemical synthesis using CO and H 2 O as raw materials at ambient conditions offers immense appeal. However, the upscaling electrosynthesis oxygenates encounters kinetic bottlenecks arising from competing hydrogen evolution reaction with selective production ethylene. Herein, catalytic relay system that can perform in tandem capture, activation, intermediate transfer enrichment on Cu-Ag composite catalyst is used for attaining high yield CO-to-oxygenates current densities. The Cu/30Ag (molar ratio Cu Ag 7:3) enables efficiency conversion, maximum partial density 800 mA cm −2 an applied 1200 , 67 % selectivity. ability finely control ethylene highlights principle efficient design based mechanism.

Language: Английский

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

239
Electrochemical C–N coupling of CO2and nitrogenous small molecules for the electrosynthesis of organonitrogen compounds DOI
Xianyun Peng, Libin Zeng, Dashuai Wang

et al.

Chemical Society Reviews, Journal Year: 2023, Volume and Issue: 52(6), P. 2193 - 2237

Published: Jan. 1, 2023

Electrochemical C–N coupling reaction by renewable electricity for the electrosynthesis of organonitrogen compounds with abundant CO 2 and nitrogenous small molecules as carbon nitrogen sources, respectively, is a promising sustainable synthetic strategy.

Language: Английский

Citations

174
Innovative Electrochemical Strategies for Hydrogen Production: From Electricity Input to Electricity Output DOI Creative Commons
Dafeng Yan, Chalachew Mebrahtu, Shuangyin Wang

et al.

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 62(16)

Published: Nov. 28, 2022

Renewable H2 production by water electrolysis has attracted much attention due to its numerous advantages. However, the energy consumption of conventional is high and mainly driven kinetically inert anodic oxygen evolution reaction. An alternative approach coupling different half-cell reactions use redox mediators. In this review, we, therefore, summarize latest findings on innovative electrochemical strategies for production. First, we address mediators utilized in splitting, including soluble insoluble species, corresponding cell concepts. Second, discuss involving organic inorganic chemical transformations. Then, at both cathode anode, or even together with electricity generation, presented. Finally, remaining challenges prospects future development research field are highlighted.

Language: Английский

Citations

117
Single‐Atom or Dual‐Atom in TiO2Nanosheet: Which is the Better Choice for Electrocatalytic Urea Synthesis? DOI
Lu Pan, Jingnan Wang, Fei Lu

et al.

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 62(8)

Published: Nov. 30, 2022

As rising star materials, single-atom and dual-atom catalysts have been widely reported in the electro-catalysis area. To answer key question: catalysts, which is better for electrocatalytic urea synthesis? we design two types of via a vacancy-anchorage strategy: Pd1 -TiO2 Cu1 nanosheets. An ultrahigh activity 166.67 molurea molPd-1 h1 with corresponding 22.54 % Faradaic efficiency at -0.5 V vs. reversible hydrogen electrode (RHE) achieved over , much higher than that . Various characterization including an situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) theoretical calculations demonstrate site more favorable producing urea, experiences C-N coupling pathway lower energy barrier compared

Language: Английский

Citations

105
Electrochemical hydrogenation and oxidation of organic species involving water DOI
Cuibo Liu, Fanpeng Chen, Bo‐Hang Zhao

et al.

Nature Reviews Chemistry, Journal Year: 2024, Volume and Issue: 8(4), P. 277 - 293

Published: March 25, 2024

Language: Английский

Citations

72
Electrocatalytic synthesis of C–N coupling compounds from CO2 and nitrogenous species DOI Creative Commons
Zheng Zhang, Danyang Li, Yunchuan Tu

et al.

SusMat, Journal Year: 2024, Volume and Issue: 4(2)

Published: March 12, 2024

Abstract The electrocatalytic synthesis of C–N coupling compounds from CO 2 and nitrogenous species not only offers an effective avenue to achieve carbon neutrality reduce environmental pollution, but also establishes a route synthesize valuable chemicals, such as urea, amide, amine. This innovative approach expands the application range product categories beyond simple carbonaceous in reduction, which is becoming rapidly advancing field. review summarizes research progress urea synthesis, using N , NO − 3 species, explores emerging trends electrosynthesis amide amine nitrogen species. Additionally, future opportunities this field are highlighted, including amino acids other containing bonds, anodic reactions water oxidation, catalytic mechanism corresponding reactions. critical captures insights aimed at accelerating development electrochemical reactions, confirming superiority method over traditional techniques.

Language: Английский

Citations

48
Indium-activated bismuth-based catalysts for efficient electrocatalytic synthesis of urea DOI Open Access

Yini Mao,

Yong Jiang,

Qiao Gou

et al.

Applied Catalysis B Environment and Energy, Journal Year: 2023, Volume and Issue: 340, P. 123189 - 123189

Published: Aug. 19, 2023

Language: Английский

Citations

45
Atomic-Scale Tailoring C–N Coupling Sites for Efficient Acetamide Electrosynthesis over Cu-Anchored Boron Nitride Nanosheets DOI
Yan Wang,

Shuai Xia,

Kui Chen

et al.

ACS Nano, Journal Year: 2024, Volume and Issue: unknown

Published: Dec. 4, 2024

Electrochemical conversion of carbon and nitrogen sources into valuable chemicals provides a promising strategy for mitigating CO

Language: Английский

Citations

36
Tandem Catalysts Enabling Efficient C−N Coupling toward the Electrosynthesis of Urea DOI

Yuhang Gao,

Jingnan Wang, Menglong Sun

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(23)

Published: April 6, 2024

Abstract The development of a methodology for synthesizing value‐added urea (CO(NH 2 ) via renewable electricity‐driven C−N coupling reaction under mild conditions is highly anticipated. However, the complex catalytic active sites that act on carbon and nitrogen species make mechanism unclear, resulting in low efficiency from co‐reduction dioxide (CO nitrate (NO 3 − ). Herein, we propose novel tandem catalyst Mo‐PCN‐222(Co), which Mo serve to facilitate reduction *NH intermediate, while Co enhance CO carbonic oxide (CO), thus synergistically promoting coupling. synthesized Mo‐PCN‐222(Co) exhibited noteworthy yield rate 844.11 mg h −1 g , alongside corresponding Faradaic 33.90 % at −0.4 V vs. reversible hydrogen electrode (RHE). By combining situ spectroscopic techniques with density functional theory calculations, demonstrate efficient attributed system *CO intermediates produced by stabilize formation *CONH intermediate. This study provides an effective avenue design synthesis catalysts electrocatalytic synthesis.

Language: Английский

Citations

34
Electrocatalytic upgrading of plastic and biomass‐derived polyols to formamide under ambient conditions DOI

Qiujin Shi,

Wengio Tang,

Kejian Kong

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: unknown

Published: June 1, 2024

Abstract Electrocatalytic upgrading of wasted plastic and renewable biomass represents a sustainable method to produce chemicals but is limited carbohydrates, leaving other value‐added chemicals, such as organonitrogen compounds, being scarcely explored. Herein, we reported an electrocatalytic oxidation strategy transform polyethylene terephthalate (PET) plastic‐derived ethylene glycol (EG) biomass‐derived polyols into formamide, in the presence ammonia (NH 3 ) over tungsten oxide (WO catalyst. Taking EG‐to‐formamide example, achieved high formamide productivity 537.7 μmol cm −2 h −1 with FE 43.2 % at constant current 100 mA flow electrolyzer 12‐h test, representing more advantageous performance compared previous reports for electrosynthesis. Mechanistic understanding revealed that cleavage C−C bond EG was facilitated by nucleophilic attack situ formed nitrogen radicals from NH , resultant C−N construction eventually production. Furthermore, this can be extended transformation PET bottle series carbon number three (glycerol) six (glucose), producing efficiencies. This work demonstrates may have implications production beyond carbohydrates.

Language: Английский

Citations

22