ACS Catalysis, Journal Year: 2025, Volume and Issue: unknown, P. 5968 - 5981
Published: March 27, 2025
Language: Английский
Advanced Energy Materials, Journal Year: 2024, Volume and Issue: unknown
Published: Aug. 13, 2024
Abstract The rational design of a photocatalyst and its microenvironmental modulation is crucial in the heterogeneous photocatalysis process, yet relevant research on photocatalytic biodiesel synthesis not explored. Herein, based prediction density functional theory (DFT) calculations, highly efficient ternary biocompatible montmorillonite (Mt) nanocomposites S‐scheme heterojunction photocatalysts (g‐C 3 N 4 ‐TiO 2 @Mt, CTM) are successfully rationally designed. By modulating microenvironment production, CTM‐2 demonstrates exceptional catalytic performance stability, achieving record‐breaking yield 98.5%. Through ex/in situ X‐ray photoelectron spectroscopy (XPS), absorption near‐edge (XANES), theoretical formation revealed, which can generate an interface electric field (IEF) that provides intrinsic driving force for carrier migration enhances surface positivity. This boosts enrichment effect electronegative oleic acid (OA) carboxyl molecules, thus greatly enriching substrate concentration improving reaction microenvironment. Moreover, fourier transform infrared spectrometer (FT‐IR)/Raman together with electron paramagnetic resonance (EPR) further confirm key intermediates CH O• ester carbonyl (C═O), DFT calculations provide reference pathway, determined to be capable significantly reducing energy barrier rate‐determining step.
Language: Английский
Citations
27
Chemical Reviews, Journal Year: 2025, Volume and Issue: unknown
Published: Feb. 18, 2025
The electrocatalytic technique, as an efficient energy storage and conversion technology, has attracted significant attention to address exhaustion environmental pollution. Usually, the activity selectivity of reactions are largely dominated by dynamic process occurring on electrocatalysts. Therefore, high-performance electrocatalysts, which can dominate pathway barrier reactions, great significance for advancement technique. Metal-organic frameworks (MOFs), emerging crystalline porous materials, present structural component advantages including well-defined structure, high surface area, large porosity, diverse components, easy tailorability, demonstrating fantastic potential precise fabrication In this Review, strategies in electrocatalysts based MOF-related materials specifically introduced from aspects catalytic site design microenvironment modulation around sites. Furthermore, representative progress achieved various applications employing MOF-based is systematically summarized, with special emphasis MOFs performance optimization. Finally, remaining challenges future perspectives further highlighted.
Language: Английский
Citations
8
Nature Communications, Journal Year: 2025, Volume and Issue: 16(1)
Published: Feb. 19, 2025
Abstract Acidic electrochemical CO 2 conversion is a promising alternative to overcome the low utilization. However, over-reliance on highly concentrated K + inhibit hydrogen evolution reaction also causes (bi)carbonate precipitation interfere with catalytic performance. In this work, under screening and guidance of computational simulations, we present carbon coated tip-like O 3 electrocatalyst for stable efficient acidic synthesize formic acid (HCOOH) concentration. The layer protects oxidized species higher intrinsic activity from reductive corrosion, peripherally formulates tip-induced electric field regulate adverse H attraction desirable enrichment. an electrolyte at pH 0.94, only 0.1 M required achieve Faradaic efficiency (FE) 98.9% 300 mA cm −2 HCOOH long-time stability over100 h. By up-scaling electrode into 25 electrolyzer setup, total current 7 A recorded sustain durable production 291.6 mmol L −1 h .
Language: Английский
Citations
3
Nano Energy, Journal Year: 2024, Volume and Issue: 130, P. 110088 - 110088
Published: Aug. 6, 2024
Electrocatalytic nitrate reduction (NitRR) offers exciting potential for mass production of ammonia (NH3) from renewables. However, the rigidity metal−ligand bonds in most electrocatalysts renders them unable to survive structural transformations required NitRR. Herein, we establish a type non-rigid metal−oxygen by employing graphene oxide (GO) sheets as 'micron-scale' ligand transition metals (TM). Because being confined interfaces between GO and TM, oxygenated groups can associate with dissociate TM response reaction dynamics. As proof-of-concept demonstration, an electrocatalyst was developed dispersing nanoscale ruthenium (Ru) on utilizing two-dimensional MXene compensate low electrical conductivity GO. This exhibits maximum NH3 yield over 5 mg cm−2 h−1, almost 100 % current-to-NH3 efficiency, far outperforming performance reported Ru-based materials. What's even more remarkable is achievement record-breaking performance: 200-hour stable electrolysis 40.2 using membrane electrode reactor. Our experimental theoretical investigations further reveal non-rigidity Ru–O how they self-regulate adapt diverse intermediates involved work provides approach fabricate high-performance featuring reversible bonds, opening new possibilities practical electrolysis.
Language: Английский
Citations
10
Advanced Energy Materials, Journal Year: 2025, Volume and Issue: unknown
Published: Feb. 5, 2025
Abstract Electrocatalytic CO 2 reduction (CO RR) is rapidly emerging as a promising sustainable strategy for transforming into valuable fuels and chemical feedstocks, crucial step toward carbon‐neutral society. The efficiency, selectivity, stability of RR are heavily influenced by the chosen catalyst operating conditions used. Despite substantial advances in development catalysts, there scarcity comprehensive reviews focusing on influence different environments performance. This review offers detailed examination internal external environmental control strategies designed to enhance efficiency. fundamental reaction mechanisms through situ operational techniques, paired with theoretical analyses, discussed while also identifying key challenges future research directions technology. By delivering overview current state field, this highlights critical role control, mechanistic insights, practical considerations needed successful commercialization
Language: Английский
Citations
2
Nature Synthesis, Journal Year: 2025, Volume and Issue: unknown
Published: March 20, 2025
Language: Английский
Citations
1
Proceedings of the National Academy of Sciences, Journal Year: 2024, Volume and Issue: 121(41)
Published: Oct. 3, 2024
Acidic CO
Language: Английский
Citations
8
Environmental 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
7
Advanced Science, Journal Year: 2025, Volume and Issue: unknown
Published: Jan. 21, 2025
Abstract Electrochemical CO 2 reduction in acidic media attracts extensive research attention due to its potential increasing carbon efficiency. In most reports, alkali cations are introduced suppress hydrogen evolution and promote reduction. However, the mass transport of through cation exchange membrane induces change electrolyte compositions. Herein, variation compositions flow during analyzed quantitatively by simulation experiments. If initial amount anolyte is higher than H + catholyte, pH catholyte increases remarkably long‐term electrolysis, resulting decrease Bicarbonate salt precipitation on cathode with cation‐containing another origin Faradaic efficiency To maintain high efficiency, should contain low concentration or even be free cations. Decorating catalyst ionomer density sites enables pure acid solution, achieving 30‐h stable
Language: Английский
Citations
1
Research, Journal Year: 2024, Volume and Issue: 8
Published: Jan. 13, 2024
The electrocatalytic carbon dioxide reduction reaction (CO2RR) at industrial-level current densities provides a sustainable approach to converting CO2 into value-added fuels and feedstocks using renewable electricity. However, the CO2RR conducted typically in alkaline neutral electrolytes encounters some challenges due inevitable between OH- ions, which undermines utilization leads poor operational stability. Acidic media present viable alternative by reducing (bi)carbonate production, thereby enhancing efficiency stability CO2RR. objective of this paper is provide concise account recent advancements field acidic CO2RR, with an emphasis on future developments opportunities.
Language: Английский
Citations
6