Multiple Reaction Pathways for Oxygen Evolution as a Key Factor for the Catalytic Activity of Nickel–Iron (Oxy)Hydroxides DOI
Giuseppe Mattioli, Leonardo Guidoni

Journal of the American Chemical Society, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 15, 2025

We present a comprehensive theoretical study, using state-of-the-art density functional theory simulations, of the structural and electrochemical properties amorphous pristine iron-doped nickel–(oxy)hydroxide catalyst films for water oxidation in alkaline solutions, referred to as NiCat Fe:NiCat. Our simulations accurately capture changes locally ordered units, reported by X-ray absorption spectroscopy, when are activated exposure positive potential. emphasize critical role proton-coupled electron transfer reversible Ni(II) Ni(III/IV) during this activation. After establishing models Fe:NiCat consistent with experimental data, we used them explore atomistic mechanism oxygen evolution reaction (OER), which is triggered once applied potential exceeds overpotential required production. quantitatively compared seven OER pathways applicable both adsorbate (AEM) lattice-oxygen-mediated (LOM) families, elucidating how iron significantly enhances catalytic activity NiCat. findings suggest that simple metal–oxygen–metal motifs, common on surface crystalline metal (oxy)hydroxide films, can promote AEM LOM mechanisms under typical conditions. Furthermore, propose elusive lies distinct behavior Ni(IV)–O Fe(IV)–O bonds key intermediates preceding formation O–O bond, Fe ions lowering needed form these across investigated pathways.

Language: Английский

Porphyrin-based metal–organic frameworks for photo(electro)catalytic CO2 reduction DOI

Guixiang Ding,

Chunxue Li, Lihui Chen

et al.

Energy & Environmental Science, Journal Year: 2024, Volume and Issue: 17(15), P. 5311 - 5335

Published: Jan. 1, 2024

The panorama of the latest developments emerging porphyrin-based MOFs for photo(electro)catalytic CO 2 reduction is shown.

Language: Английский

Citations

38
Unveiling pH‐Dependent Adsorption Strength of *CO2− Intermediate over High‐Density Sn Single Atom Catalyst for Acidic CO2‐to‐HCOOH Electroreduction DOI Creative Commons
Bin Sun,

Zaiqi Li,

Difei Xiao

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(14)

Published: Feb. 16, 2024

Abstract The acidic electrochemical CO 2 reduction reaction (CO RR) for direct formic acid (HCOOH) production holds promise in meeting the carbon‐neutral target, yet its performance is hindered by competing hydrogen evolution (HER). Understanding adsorption strength of key intermediates electrolyte indispensable to favor RR over HER. In this work, high‐density Sn single atom catalysts (SACs) were prepared and used as catalyst, reveal pH‐dependent coverage *CO − intermediatethat enables enhanced towards HCOOH production. At pH=3, SACs could deliver a high Faradaic efficiency (90.8 %) formation corresponding partial current density up −178.5 mA cm −2 . detailed situ attenuated total reflection Fourier transform infrared (ATR‐FTIR) spectroscopic studies that favorable alkaline microenvironment formed near surface SACs, even electrolyte. More importantly, intermediate unravelled which turn affects competition between HER

Language: Английский

Citations

36
Switching CO2 Electroreduction toward Ethanol by Delocalization State-Tuned Bond Cleavage DOI
Zhengzheng Liu,

Lu Song,

Ximeng Lv

et al.

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(20), P. 14260 - 14266

Published: May 7, 2024

The electrochemical CO2 reduction reaction by copper-based catalysts features a promising approach to generate value-added multicarbon (C2+) products. However, due the unfavored formation of oxygenate intermediates on catalyst surface, selectivity C2+ alcohols like ethanol remains unsatisfactory compared that ethylene. bifurcation point (i.e., CH2═CHO* intermediate adsorbed Cu via Cu–O–C linkage) is critical product selectivity, whereas subsequent cleavage Cu–O or O–C bond determines ethylene pathway. Inspired hard–soft acid–base theory, in this work, we demonstrate an electron delocalization tuning strategy nitrene surface functionalization approach, which allows weakening and cleaving CH2═CHO*, as well accelerating hydrogenation C═C along As result, nitrene-functionalized exhibited much-enhanced Faradaic efficiency 45% with peak partial current density 406 mA·cm–2, substantially exceeding unmodified amide-functionalized Cu. When assembled membrane electrode assembly electrolyzer, presented stable CO2-to-ethanol conversion for >300 h at industrial 400 mA·cm–2.

Language: Английский

Citations

36
Stabilizing the oxidation state of catalysts for effective electrochemical carbon dioxide conversion DOI

Zhitong Wang,

Lizhi Xu, Yansong Zhou

et al.

Chemical Society Reviews, Journal Year: 2024, Volume and Issue: 53(12), P. 6295 - 6321

Published: Jan. 1, 2024

Developing sophisticated strategies to stabilize oxidative metal catalysts based on the correlation between dynamic oxidation state and product profile is favorable for efficient electrochemical CO 2 conversion.

Language: Английский

Citations

34
Cooperation of Different Active Sites to Promote CO2 Electroreduction to Multi‐carbon Products at Ampere‐Level DOI

Dawei Zhou,

Chunjun Chen, Yichi Zhang

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(15)

Published: Feb. 12, 2024

Abstract Electroreduction of CO 2 to C 2+ products provides a promising strategy for reaching the goal carbon neutrality. However, achieving high selectivity at current density remains challenge. In this work, we designed and prepared multi‐sites catalyst, in which Pd was atomically dispersed Cu (Pd−Cu). It found that Pd−Cu catalyst had excellent performance producing from electroreduction. The Faradaic efficiency (FE) could be maintained approximately 80.8 %, even 0.8 A cm −2 least 20 hours. addition, FE above 70 % 1.4 . Experiments functional theory (DFT) calculations revealed three distinct catalytic sites. These active sites allowed efficient conversion , water dissociation, conversion, ultimately leading yields products.

Language: Английский

Citations

29
Selective Increase in CO2 Electroreduction to Ethanol Activity at Nanograin‐Boundary‐Rich Mixed Cu(I)/Cu(0) Sites via Enriching Co‐Adsorbed CO and Hydroxyl Species DOI
Ting Zhang,

Shenglin Xu,

De‐Li Chen

et al.

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

Published: May 31, 2024

Selective producing ethanol from CO

Language: Английский

Citations

24
Catalyst design for electrochemical CO2 reduction to ethylene DOI Creative Commons
Yuanjun Chen, Rui Kai Miao, Christine J. Yu

et al.

Matter, Journal Year: 2024, Volume and Issue: 7(1), P. 25 - 37

Published: Jan. 1, 2024

Language: Английский

Citations

23
Acetamide Electrosynthesis from CO2 and Nitrite in Water DOI
Siyu Kuang, Tian‐Tian Xiao, Haoyuan Chi

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(9)

Published: Jan. 11, 2024

Renewable electricity driven electrocatalytic CO

Language: Английский

Citations

23
Recent Advances and Challenges in Efficient Selective Photocatalytic CO2 Methanation DOI

Piyan Wang,

Fengyi Yang, Jiafu Qu

et al.

Small, Journal Year: 2024, Volume and Issue: 20(32)

Published: March 15, 2024

Abstract Solar‐driven carbon dioxide (CO 2 ) methanation holds significant research value in the context of emission reduction and energy crisis. However, this eight‐electron catalytic reaction presents substantial challenges activity selectivity. In regard, researchers have conducted extensive exploration achieved developments. This review provides an overview recent advances efficient selective photocatalytic CO methanation. It begins by discussing fundamental principles detail, analyzing strategies for improving efficiency conversion to CH 4 comprehensively. Subsequently, it outlines applications advanced characterization methods Finally, highlights prospects opportunities area, aiming inspire into high‐value shed light on mechanisms.

Language: Английский

Citations

17
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