High‐rate CO2‐to‐CH4 Electrosynthesis by Undercoordinated Cu Sites in Alkaline‐Earth‐Metal Perovskites with Strong Basicity DOI
Zikai Xu, Peng Chen, Gan Luo

et al.

Advanced Energy Materials, Journal Year: 2023, Volume and Issue: 13(19)

Published: April 9, 2023

Abstract The electrochemical CO 2 reduction to CH 4 has been extensively demonstrated, but still suffers from relatively poor activity and requires high overpotentials especially at large electrolysis rates. Perovskite oxides (A x B y O) are one type of promising electrocatalyst for the due their tunable electronic structures. In this work, a Ca CuO 3 perovskite oxide catalyst is developed with alkaline‐earth A‐sites, featuring an inherently strong basic strengthand outstanding capability adsorption, as well undercoordinated Cu sites generated through partial surface 2+ cation leaching. exhibitsa current density 517 ± 23 mA cm −2 producing low applied potential −0.30 V versus reversible hydrogen electrode, which further reached peak value 1452 156 . Density functional calculations show that allowed promote hydrogenation * subsequent CHO intermediates, thus leading activity. This work suggests attractive design strategy tuning A‐sites in realize high‐rate ‐to‐CH electrosynthesis overpotentials.

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

225

Selective electrochemical synthesis of urea from nitrate and CO2 via relay catalysis on hybrid catalysts DOI
Yuting Luo, Ke Xie, Pengfei Ou

et al.

Nature Catalysis, Journal Year: 2023, Volume and Issue: 6(10), P. 939 - 948

Published: Sept. 11, 2023

Language: Английский

Citations

151

Membrane Electrode Assembly for Electrocatalytic CO2 Reduction: Principle and Application DOI
Zheng Zhang, Xin Huang, Zhou Chen

et al.

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(28)

Published: March 27, 2023

Abstract Electrocatalytic CO 2 reduction reaction (CO RR) in membrane electrode assembly (MEA) systems is a promising technology. Gaseous can be directly transported to the cathode catalyst layer, leading enhanced rate. Meanwhile, there no liquid electrolyte between and anode, which help improve energy efficiency of whole system. The remarkable progress achieved recently points out way realize industrially relevant performance. In this review, we focus on principles MEA for RR, focusing gas diffusion electrodes ion exchange membranes. Furthermore, anode processes beyond oxidation water are considered. Besides, voltage distribution scrutinized identify specific losses related individual components. We also summarize generation different reduced products together with corresponding catalysts. Finally, challenges opportunities highlighted future research.

Language: Английский

Citations

91

Copper with an atomic-scale spacing for efficient electrocatalytic co-reduction of carbon dioxide and nitrate to urea DOI
Seokmin Shin, Siraj Sultan,

Zong-Xian Chen

et al.

Energy & Environmental Science, Journal Year: 2023, Volume and Issue: 16(5), P. 2003 - 2013

Published: Jan. 1, 2023

This work presents that Cu with atomic-scale spacings ( d s ) efficiently catalyses the electrochemical co-reduction of CO 2 and NO 3 − to urea. Specifically, near 6 Å (6 Å-Cu) produces urea a high yield rate partial current density.

Language: Английский

Citations

82

Heterogeneous electrosynthesis of C–N, C–S and C–P products using CO2 as a building block DOI
Junnan Li,

Hamed Heidarpour,

Guorui Gao

et al.

Nature Synthesis, Journal Year: 2024, Volume and Issue: 3(7), P. 809 - 824

Published: May 17, 2024

Language: Английский

Citations

27

Mind the Interface: The Role of Adsorption in Electrocatalysis DOI
Christine Lucky, Marcel Schreier

ACS Nano, Journal Year: 2024, Volume and Issue: 18(8), P. 6008 - 6015

Published: Feb. 14, 2024

In the field of electrocatalysis, significant emphasis has been placed on developing electrode materials to enable critical energy storage reactions and sustainable chemical synthesis. However, is just one part a complex interfacial environment that controls substrate adsorption reactivity. presence liquid electrolyte an electrochemical interface, processes behave substantially differently than those in gas phase. Understanding these processes, which play important role all electrocatalytic reactions, for design effective electrocatalysts. this Perspective, we discuss current understanding its implications catalyst design.

Language: Английский

Citations

19

Towards carbon-neutral biotechnologies for rural wastewater: A review of current treatment processes and future perspectives DOI
Xinzheng Zhang, Guangyi Ma, Tao Chen

et al.

Journal of Water Process Engineering, Journal Year: 2024, Volume and Issue: 58, P. 104773 - 104773

Published: Jan. 9, 2024

Language: Английский

Citations

16

The green chemistry paradigm in modern organic synthesis DOI
Sergei G. Zlotin, Ksenia S. Egorova, Valentine P. Ananikov

et al.

Russian Chemical Reviews, Journal Year: 2023, Volume and Issue: 92(12), P. RCR5104 - RCR5104

Published: Dec. 1, 2023

After the appearance of green chemistry concept, which was introduced in vocabulary early 1990s, its main statements have been continuously developed and modified. Currently, there are 10–12 cornerstones that should form basis for an ideal chemical process. This review analyzes accumulated experience achievements towards design products processes reduce or eliminate use generation hazardous substances. The presents views leading Russian scientists specializing various fields this subject, including homogeneous heterogeneous catalysis, fine basic organic synthesis, electrochemistry, polymer chemistry, based on bio-renewable feedstocks energetic compounds materials. A new approach to quantitative evaluation environmental friendliness by authors is described. <br> bibliography includes 1761.

Language: Английский

Citations

39

Electrochemical Wastewater Refining: A Vision for Circular Chemical Manufacturing DOI
Dean M. Miller,

Kristen Abels,

Jinyu Guo

et al.

Journal of the American Chemical Society, Journal Year: 2023, Volume and Issue: 145(36), P. 19422 - 19439

Published: Aug. 29, 2023

Wastewater is an underleveraged resource; it contains pollutants that can be transformed into valuable high-purity products. Innovations in chemistry and chemical engineering will play critical roles valorizing wastewater to remediate environmental pollution, provide equitable access resources services, secure materials from diminishing feedstock availability. This perspective envisions electrochemical refining─the use of processes tune recover specific products wastewaters─as the necessary framework accelerate wastewater-based electrochemistry widespread practice. We define prescribe a use-informed approach simultaneously serves wastewater-pollutant-product triads uncovers mechanistic understanding generalizable broad cases. this evaluate research needs case studies electrocatalysis, stoichiometric conversions, separations. Finally, we rationale guidance for intentionally expanding refining product portfolio. require coordinated effort multiple expertise areas meet urgent need extracting maximal value complex, variable, diverse, abundant resources.

Language: Английский

Citations

38

Understanding the Oxidative Properties of Nickel Oxyhydroxide in Alcohol Oxidation Reactions DOI Creative Commons
Petrus C. M. Laan, Felix J. de Zwart, Emma Wilson

et al.

ACS Catalysis, Journal Year: 2023, Volume and Issue: 13(13), P. 8467 - 8476

Published: June 12, 2023

The NiOOH electrode is commonly used in electrochemical alcohol oxidations. Yet understanding the reaction mechanism far from trivial. In many cases, difficulty lies decoupling of overlapping influence chemical and factors that not only govern pathway but also crystal structure situ formed oxyhydroxide. Here, we use a different approach to understand this system: start with synthesizing pure forms two oxyhydroxides, β-NiOOH γ-NiOOH. Then, using oxidative dehydrogenation three typical alcohols as model reactions, examine reactivity selectivity each While solvent has clear effect on rate β-NiOOH, observed was found be unaffected remained over 95% for both primary secondary aldehydes ketones, respectively. Yet, high concentration OH- aqueous promoted preferential conversion benzyl benzoic acid. Thus, formation carboxylic compounds oxidation without alkaline electrolyte more likely follow direct pathway. Overoxidation β- γ-phase will affect sustained >95% conversion. mechanistic examinations comprising kinetic isotope effects, Hammett analysis, spin trapping studies reveal oxidatively dehydrogenated benzaldehyde via consecutive hydrogen atom transfer steps. This work offers unique catalytic properties shedding light NiOOH-based electrodes.

Language: Английский

Citations

28