Efficient Electroreduction of CO2 to Formate via Simultaneous Tuning of Hydroxyl Group Coverage and Oxygen Vacancy Amount of In2O3 DOI
Liang Fu, Zhenping Qu,

Ling-Ling Zhou

и другие.

ACS Sustainable Chemistry & Engineering, Год журнала: 2024, Номер unknown

Опубликована: Дек. 12, 2024

Electrochemical CO2 reduction (ECR) to high value-added feedstocks is a sustainable way address energy and environmental issues. However, there still exists bottleneck in comprehending the structure–activity relationship of catalysts for ECR. Herein, we demonstrated that simultaneous tuning surface-adsorbed hydroxyl group (OHad) coverage oxygen vacancy (OV) amount on In2O3 surface was an effective approach derive excellent formate Faradaic efficiency (FE) above 80% at wide potential range from −1.0 −1.5 V versus reversible hydrogen electrode (vs RHE) with promising durability. experiments theoretical analyses revealed synergistic effect OHad OV could smartly optimize adsorption sites, accelerate electron transfer, stabilize *CO2•– *OCHO intermediates, thus facilitate ECR activity. This result will contribute understanding critical role these species ECR, which can offer valuable insights into rational catalyst design comprehensive utilization efficiency.

Язык: Английский

Tailoring CO2 Adsorption Configuration with Spatial Confinement Switches Electroreduction Product from Formate to Acetate DOI

Hua‐Qin Wang,

Heyu Sui,

Ya-Long Ding

и другие.

Journal of the American Chemical Society, Год журнала: 2025, Номер unknown

Опубликована: Фев. 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.

Язык: Английский

Процитировано

4
Electrochemical CO2 Reduction: Advances, Insights, Challenges, and Future Directions DOI Creative Commons
Asghar Ali, Muhammad Qasim, S. Sakhi

и другие.

Materials Today Sustainability, Год журнала: 2025, Номер unknown, С. 101089 - 101089

Опубликована: Фев. 1, 2025

Язык: Английский

Процитировано

2
Tip carbon encapsulation customizes cationic enrichment and valence stabilization for low K+ acidic CO2 electroreduction DOI Creative Commons

Zhitong Wang,

Dongyu Liu,

Chenfeng Xia

и другие.

Nature Communications, Год журнала: 2025, Номер 16(1)

Опубликована: Фев. 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 .

Язык: Английский

Процитировано

2
Synergistic Catalysis in Fe─In Diatomic Sites Anchored on Nitrogen‐Doped Carbon for Enhanced CO2 Electroreduction DOI Open Access
Dapeng Meng, Jingxuan Zheng, Junxin Guo

и другие.

Small, Год журнала: 2025, Номер unknown

Опубликована: Янв. 31, 2025

Diatomic catalysts are promising for the electrochemical CO2 reduction reaction (CO2RR) due to their maximum atom utilization and presence of multiple active sites. However, atomic-scale design diatomic elucidation synergistic catalytic mechanisms between centers remain challenging. In this study, heteronuclear Fe─In sites anchored on nitrogen-doped carbon (FeIn DA/NC) constructed. The FeIn DA/NC electrocatalyst achieves a CO Faradaic efficiency exceeding 90% across wide range applied potentials from -0.4 -0.7 V, with peak 99.1% at -0.5 V versus reversible hydrogen electrode. situ, attenuated total reflection surface-enhanced infrared absorption spectroscopy density functional theory calculations reveal that interaction Fe induce an asymmetric charge distribution, which promote adsorption site lowered energy barrier formation *COOH. Moreover, unique structure increase *OH through bridging interaction, decrease water dissociation further promoted CO2RR activity.

Язык: Английский

Процитировано

1
A Review on Single Site Catalysts for Electrochemical CO2 Reduction DOI
Fan Yang, Haoyu Han,

Hailong Duan

и другие.

Advanced Energy Materials, Год журнала: 2025, Номер unknown

Опубликована: Март 18, 2025

Abstract Single site catalysts (SSCs), characterized by high atomic utilization and well‐defined active sites, exhibit significant potential in the field of CO 2 electroreduction (CO RR). Typically, SSCs tend to a 2‐electron transfer reaction RR, there remain challenges achieving efficient conversion above 2‐electrons (methane (CH 4 ) multicarbon products(C 2+ ). Therefore, systematic review is crucial summarize recent advancements single electrocatalysts their structure‐activity relationship. The discussion begins with state‐of‐the‐art characterization techniques SSCs. Then influence central atoms, coordination environments, support metal‐support interactions on catalytic performance discussed detail. Subsequently, regulation strategies improve activity selectivity CH C products are discussed. Furthermore, dynamic evolution metal sites true nature during RR also addressed. Finally, associated for product formation analyzed.

Язык: Английский

Процитировано

0
Research progress on the reaction mechanism, metal-based catalysts, and reactors for CO2 electroreduction to formic acid/formate DOI

Huichang Liang,

Yankun Li, Zhichao Miao

и другие.

Journal of environmental chemical engineering, Год журнала: 2025, Номер unknown, С. 116547 - 116547

Опубликована: Апрель 1, 2025

Язык: Английский

Процитировано

0
Covalently Modified Electrode with Bismuth Nanoparticles Encapsulated in Ultrathin Porous Organic Polymer Linked by Amine Bonding for Efficient CO2 Electroreduction DOI
Li Cui, Yan Wang, Changjiang Wang

и другие.

ACS Applied Materials & Interfaces, Год журнала: 2025, Номер unknown

Опубликована: Апрель 23, 2025

Bismuth-based materials in electrocatalytic CO2 reduction (CO2RR) usually face the problem of high overpotential. We first show a covalently modified electrode with Bi nanoparticles encapsulated ultrathin porous organic polymer nanosheets (POPs) amine linkages to effectively reduce overpotential for CO2-to-formate conversion, which exhibits formate Faradaic efficiency (FEHCOO-) 98.5% and partial current density up 148.7 mA cm-2 at -0.85 V comparison that bare bismuth FEHCOO- 85% -1.15 (versus reversible hydrogen electrode). Different from reaction mechanism *CO2•- radicals as intermediate over sites, situ spectroscopic studies functional theory calculations reveal abundant POPs backbone provide chemisorption sites interact enriched molecules form carbamates (*[-NCOO-]) intermediates low barrier 0.064 eV, significantly reduces free energy conversion process formate. Moreover, promote water dissociation subsequent protonation on surface reduced -0.31 eV than 0.11 eV. This work not only delivers new but also offers clean platform investigate influence modification.

Язык: Английский

Процитировано

0
Asymmetric CO–CHO Coupling over Pr Single-Atom Alloy Enables Industrial-Level Electrosynthesis of Ethylene DOI
Yanteng Xiao, Fuqing Yu,

Chenfeng Xia

и другие.

Journal of the American Chemical Society, Год журнала: 2025, Номер unknown

Опубликована: Апрель 24, 2025

The electrocatalytic conversion of carbon dioxide (CO2) to ethylene (C2H4) holds great promise for sustainable chemical synthesis, yet achieving industrially relevant production rates remains a significant challenge. Through computational screening, we have identified praseodymium (Pr) single-atom alloy embedded in copper (Cu) catalyst (Pr@Cu) that exhibits superior CO2 activation and remarkably low energy barrier asymmetric *CO-*CHO coupling, primarily by facilitating the *CHO intermediate formation. Our optimized catalyst, Pr@Cu-2 (6 wt % Pr), achieves C2H4 Faradaic efficiency (FE) 64.2% at -1.6 V versus reversible hydrogen electrode (RHE) under high current density 1200 mA cm-2 reduction reaction (CO2RR). Furthermore, when integrated into 100 cm2 membrane assembly (MEA) electrolyzer, demonstrates robust performance, maintaining continuous rate 21.3 mL min-1 20 A over 200 h. This work provides fundamental insights role Pr alloys CO2RR highlights their potential scalable electrosynthesis.

Язык: Английский

Процитировано

0
Reversible Li2C2O4 product regulation in Li–CO2 batteries using single-atom alloy engineering DOI
Xinxin Zhang, Yu Wang, Yafei Li

и другие.

Science China Chemistry, Год журнала: 2025, Номер unknown

Опубликована: Янв. 3, 2025

Язык: Английский

Процитировано

0
Morphology Effect of Puffball Spores on Hemostasis: A Promising Solution for Hemostatic Challenges DOI Creative Commons

Xuechang Pei,

Yue Feng, Yanru Wu

и другие.

Advanced Science, Год журнала: 2025, Номер unknown

Опубликована: Фев. 28, 2025

Abstract Hemostatic materials play a crucial role in wound healing by promoting blood concentration or releasing procoagulant factors. While hydrophilic hemostatic are effective, they may cause excessive loss and difficulty removing from the wound. Conversely, hydrophobic avoid these issues but hinder release of factors due to their water‐repellent nature. This study investigates properties underlying mechanism puffball ( Bovistella sp.) spores, traditional material. The unique hollow ball‐rod morphology strong water affinity spores enable efficient removal, leading improved clotting without drawbacks typically associated with materials. Further analysis reveals that nano‐protrusions on spore surface create textured pinning effect, which prevents adhesion after clotting. Overall, exhibit efficacy comparable commercial agent QuikClot, enhanced safety reduced side effects. Their characteristic morphology, physicochemical properties, chemical compositions offer inspiration for advancing addressing current challenges healing. Additionally, this work provides new perspectives insight into pharmacological substance basis medicine, expanding beyond conventional component‐focused mentality material‐based insight.

Язык: Английский

Процитировано

0