Fuel, Journal Year: 2025, Volume and Issue: 392, P. 134877 - 134877
Published: March 1, 2025
Language: Английский
Fuel, Journal Year: 2025, Volume and Issue: 392, P. 134877 - 134877
Published: March 1, 2025
Language: Английский
Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 63(7)
Published: Dec. 28, 2023
Abstract Modulating the microenvironment of single‐atom catalysts (SACs) is critical to optimizing catalytic activity. Herein, we innovatively propose a strategy improve local reaction environment Ru single atoms by precisely switching crystallinity support from high crystalline and low crystalline, which significantly improves hydrogen evolution (HER) The catalyst anchored on low‐crystalline nickel hydroxide (Ru−LC−Ni(OH) 2 ) reconstructs distribution balance interfacial ions due activation effect metal dangling bonds support. Single‐site with oxidation state induces aggregation hydronium (H 3 O + ), leading formation acidic in alkaline media, breaking pH‐dependent HER As comparison, high‐crystalline (Ru−HC−Ni(OH) exhibits sluggish Volmer step conventional environment. expected, Ru−LC−Ni(OH) requires overpotentials 9 136 mV at 10 1000 mA cm −2 conditions operates stably 500 for h an seawater anion exchange membrane (AEM) electrolyzer. This study provides new perspective constructing highly active electrocatalysts.
Language: Английский
Citations
44eScience, Journal Year: 2024, Volume and Issue: 4(3), P. 100246 - 100246
Published: Feb. 2, 2024
Indium-based oxides are promising electrocatalysts for producing formate via CO2 reduction reaction, in which *OCHO is considered the key intermediate. Here, we identified that *COOH pathway could be preferential to produce on In2O3 of In/In2O3 heterojunction due synergistic effect oxygen species and vacancy. Specifically, *CO2 were observed related production by situ Raman spectroscopy. The theoretical calculations further demonstrated energy barrier formation was decreased presence vacancy, similar or lower than In surface. As a result, selectivity over 90% obtained prepared with 343 ± 7 mA cm–2 partial current density. Furthermore, when using Si-based photovoltaic as an supplier, 10.11% solar–to–fuel efficiency achieved.
Language: Английский
Citations
19Journal of the American Chemical Society, Journal Year: 2025, Volume and Issue: unknown
Published: Feb. 5, 2025
Multi-proton-coupled electron transfer, multitudinous intermediates, and unavoidable competing hydrogen evolution reaction during CO2 electroreduction make it tricky to control high selectivity for specific products. Here, we present spatial confinement of Fe single atoms (FeN2S2) by adjacent FeS clusters (Fe4S4) orientate the transition adsorption configuration from C,O-side O-end, which triggers a shift activated first-step protonation C–C coupling, thus switching target product HCOOH in Faraday efficiency (FE: 90.6%) on FeN2S2 CH3COOH 82.3%) Fe4S4/FeN2S2. The strength *OCHO upon solitary site is linearly related coordination number Fe–S, with predominantly produced over single-atom (ortho-substituted S atoms). Fe4S4 cluster functions as switch reduction product, can not only optimize electronic structure neighboring but also impel complete hydrocarbon intermediate *CH3, followed coupling CO2* *CH3 via synergistic catalysis This strategy provides new avenue modulate reactant model desirable pathways, potential applications diverse multistep electrochemical processes controlled selectivity.
Language: Английский
Citations
4Advanced Energy Materials, Journal Year: 2023, Volume and Issue: 13(47)
Published: Nov. 2, 2023
Abstract The electrochemical CO 2 (eCO )‐to‐multicarbon conversion with higher value is regarded as a potential way to promote the transformation of industrial production and green balance carbon cycle. Recently, series advances have been achieved in progress eCO ‐to‐multicarbon conversion, including in‐depth exploration coupling mechanisms, up‐to‐date development characterization techniques, novel interdisciplinary design strategies catalysts electrolytic systems. Therefore, it essential systematically overview from fundamentals industrialization, compensating for limited insufficient reviews that reported. To fill aforementioned research gap, this focused on industrialization. First, possible catalytic mechanisms are accordingly summarized order reduction, small molecule‐coupled tandem conversion. Second, situ technologies assisting rationalization presented. Third, optimizing systems briefly classified advance industrialization process. Finally, challenges perspectives further reasonably proposed, aiming offer insights following work field.
Language: Английский
Citations
31Angewandte Chemie, Journal Year: 2023, Volume and Issue: 136(7)
Published: Dec. 28, 2023
Abstract Modulating the microenvironment of single‐atom catalysts (SACs) is critical to optimizing catalytic activity. Herein, we innovatively propose a strategy improve local reaction environment Ru single atoms by precisely switching crystallinity support from high crystalline and low crystalline, which significantly improves hydrogen evolution (HER) The catalyst anchored on low‐crystalline nickel hydroxide (Ru−LC−Ni(OH) 2 ) reconstructs distribution balance interfacial ions due activation effect metal dangling bonds support. Single‐site with oxidation state induces aggregation hydronium (H 3 O + ), leading formation acidic in alkaline media, breaking pH‐dependent HER As comparison, high‐crystalline (Ru−HC−Ni(OH) exhibits sluggish Volmer step conventional environment. expected, Ru−LC−Ni(OH) requires overpotentials 9 136 mV at 10 1000 mA cm −2 conditions operates stably 500 for h an seawater anion exchange membrane (AEM) electrolyzer. This study provides new perspective constructing highly active electrocatalysts.
Language: Английский
Citations
28Coordination Chemistry Reviews, Journal Year: 2024, Volume and Issue: 508, P. 215775 - 215775
Published: March 14, 2024
Language: Английский
Citations
12Chemical Reviews, Journal Year: 2024, Volume and Issue: 124(21), P. 12006 - 12085
Published: Oct. 31, 2024
Catalytic COx (CO and CO2) hydrogenation to valued chemicals is one of the promising approaches address challenges in energy, environment, climate change. H2O an inevitable side product these reactions, where its existence effect are often ignored. In fact, significantly influences catalytic active centers, reaction mechanism, performance, preventing us from a definitive deep understanding on structure-performance relationship authentic catalysts. It necessary, although challenging, clarify provide practical strategies tune concentration distribution optimize influence. this review, we focus how induces structural evolution catalysts assists processes, as well efforts understand underlying mechanism. We summarize discuss some representative tuning for realizing rapid removal or local enrichment around catalysts, along with brief techno-economic analysis life cycle assessment. These fundamental understandings further extended reactions CO CO2 reduction under external field (light, electricity, plasma). also present suggestions prospects deciphering controlling applications.
Language: Английский
Citations
11Journal of Energy Chemistry, Journal Year: 2025, Volume and Issue: unknown
Published: Jan. 1, 2025
Language: Английский
Citations
1Coordination Chemistry Reviews, Journal Year: 2025, Volume and Issue: 533, P. 216541 - 216541
Published: Feb. 28, 2025
Language: Английский
Citations
1Applied Catalysis B Environment and Energy, Journal Year: 2023, Volume and Issue: 340, P. 123281 - 123281
Published: Sept. 9, 2023
Language: Английский
Citations
17