Science China Chemistry, Год журнала: 2024, Номер unknown
Опубликована: Дек. 25, 2024
Язык: Английский
Nature Reviews Materials, Год журнала: 2024, Номер 9(9), С. 643 - 656
Опубликована: Июль 31, 2024
Язык: Английский
Процитировано
32
Advanced Materials, Год журнала: 2024, Номер 36(27)
Опубликована: Апрель 17, 2024
Abstract Ordered pore engineering that embeds uniform pores with periodic alignment in electrocatalysts opens up a new avenue for achieving further performance promotion. Hierarchically ordered porous metal–organic frameworks (HOP‐MOFs) possessing multilevel distribution are the promising precursors exploration of electrocatalysts, while scalable acquisition HOP‐MOFs editable components and adjustable size regimes is critical. This review presents recent progress on hierarchically MOF‐based materials enhanced electrocatalysis. The synthetic strategies different regimes, including self‐assembly guided by reticular chemistry, surfactant, nanoemulsion, nanocasting, first introduced. Then applications as exploring summarized, selecting representatives to highlight boosted performance. Especially, intensification molecule ion transport integrated optimized electron transfer site exposure over derivatives emphasized clarify directional integration effect endowed engineering. Finally, remaining scientific challenges an outlook this field proposed. It hoped will guide nanocatalysts boosting catalytic promoting practical applications.
Язык: Английский
Процитировано
29
Angewandte Chemie International Edition, Год журнала: 2024, Номер unknown
Опубликована: Июль 18, 2024
Abstract Single Fe sites have been explored as promising catalysts for the CO 2 reduction reaction to value‐added CO. Herein, we introduce a novel molten salt synthesis strategy developing axial nitrogen‐coordinated Fe‐N 5 on ultrathin defect‐rich carbon nanosheets, aiming modulate pathway precisely. This distinctive architecture weakens spin polarization at sites, promoting dynamic equilibrium of activated intermediates and facilitating balance between *COOH formation *CO desorption active site. Notably, synthesized FeN , supported in nitrogen‐doped (FeN @DNC), exhibits superior performance RR, achieving Faraday efficiency 99 % production (−0.4 V vs. RHE) an H‐cell, maintaining 98 current density 270 mA cm −2 (−1.0 flow cell. Furthermore, @DNC catalyst is assembled reversible Zn−CO battery with cycle durability 24 hours. In situ IR spectroscopy functional theory (DFT) calculations reveal that N coordination traction induces transformation crystal field local symmetry, therefore weakening central atom lowering energy barrier desorption.
Язык: Английский
Процитировано
11
Small, Год журнала: 2025, Номер unknown
Опубликована: Март 28, 2025
Abstract The primary hurdle faced in the practical application of proton exchange membrane water electrolyzer (PEMWE) involves improving intrinsic kinetic activity oxygen evolution reaction (OER) electrocatalysts while concurrently enhancing their durability. Although based on lattice oxygen‐mediated mechanism (LOM) have potential to significantly enhance OER without being restricted by scaling relationships, they are neglected acidic electrolytes due limited In this study, an innovative approach is presented simultaneously promote activation and improve durability LOM‐based incorporating d 0 metal ions into RuO 2 electrocatalyst. Leveraging unique electronic properties ion, O 2p band center Ru‐O covalency electrocatalyst successfully engineered, resulting change mechanism. Furthermore, a single cell PEMWE, demonstrates outstanding performance, achieving 3.0 A cm −2 at 1.81 V maintaining for 100 h 200 mA , surpassing commercial . This strategy challenges traditional viewpoint that suppressing essential PEMWE durability, offering new perspectives development electrolytes.
Язык: Английский
Процитировано
1
Advanced Energy Materials, Год журнала: 2024, Номер unknown
Опубликована: Июнь 11, 2024
Abstract The electrochemical carbon dioxide reduction reaction (CO 2 RR) is a promising approach for reducing atmospheric ) emissions, allowing harmful CO to be converted into more valuable carbon‐based products. On one hand, single (C 1 products have been obtained with high efficiency and show great promise industrial capture. However, multi‐carbon 2+ possess market value demonstrated significant as potential RR. Due RR's multiple pathways similar equilibrium potentials, the extended mechanisms necessary form C continue reduce overall selectivity of ‐to‐C electroconversion. Meanwhile, RR whole faces many challenges relating system optimization, owing an intolerance low surface pH, systemic stability utilization issues, competing side in H evolution (HER). Ethylene 4 remains incredibly within chemical industry; however, current established method producing ethylene (steam cracking) contributes emission atmosphere. Thus, strategies significantly increase this technology are essential. This review will discuss vital factors influencing forming summarize recent advancements electrosynthesis.
Язык: Английский
Процитировано
8
Angewandte Chemie International Edition, Год журнала: 2025, Номер unknown
Опубликована: Март 10, 2025
Relay catalysis represents significant efficacy in alleviating competition among different reactants during coupling reactions. However, a comprehensive understanding of the reaction mechanism underlying relay for urea electrosynthesis remains challenging. Herein, we have developed catalyst (CuAC-CuSA@NC) comprising Cu atomic clusters (CuAC) with satellite Cu─N4 single atoms (CuSA) sites on nitrogen-doped porous interconnected carbon skeleton (NC), enabling elucidation process co-reduction CO2 and NO3 -. The designed CuAC-CuSA@NC exhibits an approximately threefold higher yield rate compared to that CuSA@NC at -1.3 V versus RHE. Ex-situ experimental results in-situ attenuated total reflection surface-enhanced infrared absorption spectroscopy analysis reveal formation sequence between *NH2 *NH2CO species increasing reduction potential. combination theoretical calculations further elucidates pathway involves "CuAC" facilitating conversion *NO3 *NOx, followed by hydrogenation form *H from water dissociation promoted "CuSA" sites, which subsequently couples *CO2 produce urea. This work provides novel insights into investigation reactions, but not limit to, synthesis.
Язык: Английский
Процитировано
1
ACS Catalysis, Год журнала: 2024, Номер 14(21), С. 16224 - 16233
Опубликована: Окт. 18, 2024
Revealing the synergistic catalytic mechanism involving multiple active centers is crucial for understanding multiphase catalysis. However, complex structures of catalysts and interfacial environments pose a challenge in thoroughly exploring experimental evidence. This study reports utilization CuNi dual-atom catalyst (Cu/Ni–NC) electrochemical reduction CO2. It demonstrates high Faradaic efficiency CO exceeding 99%, remarkable reaction activity with partial current density surpassing –300 mA cm–2, prolonged stability more than 5 days at –200 mA·cm–2. Operando characterization techniques functional theory calculations reveal that Ni atoms function as sites activation hydrogenation CO2, while Cu serve dissociation H2O, supplying protons subsequent process. Moreover, electronic interactions between facilitate formation *COOH illustrating CO2 sites.
Язык: Английский
Процитировано
6
Angewandte Chemie, Год журнала: 2024, Номер 136(43)
Опубликована: Июль 18, 2024
Abstract Single Fe sites have been explored as promising catalysts for the CO 2 reduction reaction to value‐added CO. Herein, we introduce a novel molten salt synthesis strategy developing axial nitrogen‐coordinated Fe‐N 5 on ultrathin defect‐rich carbon nanosheets, aiming modulate pathway precisely. This distinctive architecture weakens spin polarization at sites, promoting dynamic equilibrium of activated intermediates and facilitating balance between *COOH formation *CO desorption active site. Notably, synthesized FeN , supported in nitrogen‐doped (FeN @DNC), exhibits superior performance RR, achieving Faraday efficiency 99 % production (−0.4 V vs. RHE) an H‐cell, maintaining 98 current density 270 mA cm −2 (−1.0 flow cell. Furthermore, @DNC catalyst is assembled reversible Zn−CO battery with cycle durability 24 hours. In situ IR spectroscopy functional theory (DFT) calculations reveal that N coordination traction induces transformation crystal field local symmetry, therefore weakening central atom lowering energy barrier desorption.
Язык: Английский
Процитировано
4
ACS Nano, Год журнала: 2024, Номер unknown
Опубликована: Ноя. 1, 2024
Single-atom catalysts are promising for electrocatalytic CO2 conversion but face challenges in controllable syntheses. Herein, a facile selenic acid etching-assisted strategy has been developed to fabricate hybrid metal-semimetal dual single-atom catalyst reduction. This enables the simultaneous generation of monodisperse active sites and hierarchical morphologies with hollow nanostructures. The as-obtained Fe–Se supported by porous nitrogen-doped carbon (FeSe-NC) shows exceptional catalytic activity CO selectivity, delivering Faradaic efficiency (FE) >97% industrially comparable jCO, superior Fe catalyst. Moreover, FeSe-NC-based rechargeable Zn-CO2 battery delivers high power density (2.01 mW cm–2) outstanding FECO (>90%), as well excellent cycling stability. Experimental results together theoretical calculations reveal that etching-induced defects Se-modulated centers asymmetrical polarized charge distributions synergistically facilitate key intermediate *CO desorption thus accelerate CO2-to-CO conversion.
Язык: Английский
Процитировано
4
Inorganic Chemistry, Год журнала: 2024, Номер unknown
Опубликована: Ноя. 17, 2024
Metal-organic frameworks (MOFs) with a large number of active sites and high porosity are considered to be good platforms for the carbon dioxide electroreduction reaction (CO
Язык: Английский
Процитировано
3