Science China Chemistry, Journal Year: 2025, Volume and Issue: unknown
Published: April 28, 2025
Language: Английский
Science China Chemistry, Journal Year: 2025, Volume and Issue: unknown
Published: April 28, 2025
Language: Английский
Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(32)
Published: May 27, 2024
Abstract The practical application of the electrocatalytic CO 2 reduction reaction (CO RR) to form formic acid fuel is hindered by limited activation molecules and lack universal feasibility across different pH levels. Herein, we report a doping‐engineered bismuth sulfide pre‐catalyst (BiS‐1) that S partially retained after electrochemical reconstruction into metallic Bi for RR formate/formic with ultrahigh performance wide range. best BiS‐1 maintains Faraday efficiency (FE) ~95 % at 2000 mA cm −2 in flow cell under neutral alkaline solutions. Furthermore, catalyst shows unprecedentedly high FE (~95 %) current densities from 100 1300 acidic Notably, density can reach 700 while maintaining above 90 membrane electrode assembly electrolyzer operate stably 150 h 200 . In situ spectra functional theory calculations reveals doping modulates electronic structure effectively promotes formation HCOO* intermediate generation. This work develops efficient stable electrocatalysts sustainable production.
Language: Английский
Citations
17Desalination, Journal Year: 2025, Volume and Issue: unknown, P. 118580 - 118580
Published: Jan. 1, 2025
Language: Английский
Citations
2Advanced Energy Materials, Journal Year: 2024, Volume and Issue: 14(32)
Published: May 23, 2024
Abstract The co‐electroreduction of CO 2 and NO x ⁻ (NO 3 ⁻/NO ⁻) to generate formamide (HCONH ) offers an opportunity for downstream chemical polymer manufacturing decarbonization; however, significant challenges lie in the C‒N coupling associated low product selectivity. Herein, p ‐block metal oxides are incorporated copper provide more accessible active sites reactant adsorption activation, tuning reaction selectivity toward production. Through situ Raman synchrotron‐based infrared spectroscopy measurements, C─N bond formation is demonstrated real‐time with CuO /BiO catalyst, where detected via a *CHO *NH intermediates formation, agreement density functional theory calculations. When tested flow electrolyzer, yield rate 134 ± 11 mmol h −1 g cat reported, first report beyond conventional H‐cell measurements. These new insights on mechanisms scale‐up capability directions further development electrocatalysts
Language: Английский
Citations
15Results in Surfaces and Interfaces, Journal Year: 2024, Volume and Issue: unknown, P. 100381 - 100381
Published: Dec. 1, 2024
Language: Английский
Citations
15Materials Today, Journal Year: 2024, Volume and Issue: 76, P. 94 - 109
Published: June 6, 2024
Language: Английский
Citations
8ACS Catalysis, Journal Year: 2024, Volume and Issue: 14(11), P. 8353 - 8365
Published: May 14, 2024
Electrochemical CO2 reduction (CO2R) to formate is an attractive carbon emissions mitigation strategy due the existing market and price for formic acid. Tin effective electrocatalyst CO2R formate, but underlying reaction mechanism whether active phase of tin metallic or oxidized during openly debated. In this report, we used grand-canonical density functional theory attenuated total reflection surface-enhanced infrared absorption spectroscopy identify differences in vibrational signatures surface species on fully surfaces. Our results show that feasible both tin. We propose key difference between each termination catalyzed by surfaces limited electrochemical activation CO2, whereas slow reductive desorption formate. While exact degree oxidation unlikely be either oxidized, study highlights limiting behavior these two lays out features our predict will promote rapid catalysis. Additionally, highlight power integrating high-fidelity quantum mechanical modeling spectroscopic measurements elucidate intricate electrocatalytic pathways.
Language: Английский
Citations
7Chinese Journal of Structural Chemistry, Journal Year: 2024, Volume and Issue: 43(8), P. 100346 - 100346
Published: May 21, 2024
Language: Английский
Citations
6Angewandte Chemie, Journal Year: 2024, Volume and Issue: 136(32)
Published: May 27, 2024
Abstract The practical application of the electrocatalytic CO 2 reduction reaction (CO RR) to form formic acid fuel is hindered by limited activation molecules and lack universal feasibility across different pH levels. Herein, we report a doping‐engineered bismuth sulfide pre‐catalyst (BiS‐1) that S partially retained after electrochemical reconstruction into metallic Bi for RR formate/formic with ultrahigh performance wide range. best BiS‐1 maintains Faraday efficiency (FE) ~95 % at 2000 mA cm −2 in flow cell under neutral alkaline solutions. Furthermore, catalyst shows unprecedentedly high FE (~95 %) current densities from 100 1300 acidic Notably, density can reach 700 while maintaining above 90 membrane electrode assembly electrolyzer operate stably 150 h 200 . In situ spectra functional theory calculations reveals doping modulates electronic structure effectively promotes formation HCOO* intermediate generation. This work develops efficient stable electrocatalysts sustainable production.
Language: Английский
Citations
6Environmental Science & Technology, Journal Year: 2024, Volume and Issue: 58(25), P. 10881 - 10896
Published: June 11, 2024
One of the most promising approaches to address global challenge climate change is electrochemical carbon capture and utilization. Solid electrolytes can play a crucial role in establishing chemical-free pathway for CO2. Furthermore, they be applied electrocatalytic CO2 reduction reactions (CO2RR) increase utilization, produce high-purity liquid chemicals, advance hybrid electro-biosystems. This review article begins by covering fundamentals processes capture, emphasizing advantages utilizing solid electrolytes. Additionally, it highlights recent advancements use polymer electrolyte or layer CO2RR with multiple functions. The also explores avenues future research fully harness potential electrolytes, including integration performance assessment under realistic conditions. Finally, this discusses opportunities challenges, aiming contribute establishment green sustainable society through valorization.
Language: Английский
Citations
6Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(25), P. 17377 - 17383
Published: June 13, 2024
A prominent feature of modern electrochemical technologies, such as fuel cells and electrolysis, is the employing polyelectrolytes instead liquid electrolytes. Unlike well-studied electrode/liquid electrolyte interfaces, however, catalytic characteristics electrode/polyelectrolyte interfaces remain largely unexplored, mostly due to lack reliable probing methods. Herein, we report a universally applicable approach investigating electrocatalytic reactions at under normal conditions. By coating thin layer anion-exchange membrane (AEM) onto electrode surface, solutions with bulky organic cations were well separated, thus pure interface can be established in regular setup studied using situ spectroscopies, e.g., attenuated total reflectance surface-enhanced infrared absorption spectroscopy (ATR-SEIRAS). We found that blank Au surface was inert toward CO2 reduction reaction (CO2RR) absence alkali metal cations, whereas an AEM dramatically turn on activity. ATR-SEIRAS revealed hydrogen bond network water Au/AEM enhanced comparison which facilitated hydrogenation process CO2RR. These findings further our fundamental understanding behavior benefit development relevant technologies.
Language: Английский
Citations
6