Ceria -Mediated Dynamic Sn0/Snδ+ Redox Cycle for CO2 Electroreduction DOI
Hai Liu, Boyang Li, Zhihui Liu

и другие.

ACS Catalysis, Год журнала: 2023, Номер 13(7), С. 5033 - 5042

Опубликована: Март 29, 2023

Electrocatalytic CO2 reduction has been considered an effective carbon neutrality as well energy storage strategy integrated with renewable electricity. conversion to formate is a feasible route using earth-abundant and nontoxic tin-based catalysts. However, they suffer from degradation thus decrease in selectivity during operation. Guided by density functional theory (DFT) calculations, herein, we synthesized CeO2–SnO2 heterostructures facile electrospinning method, which exhibited maximum partial current of ∼500 mA·cm–2 87.1% faradaic efficiency long-term stability flow cell. Proved situ attenuated total reflectance infrared absorption spectroscopy (ATR-IRAS) Raman spectra post-X-ray photoelectron (XPS) analysis, dynamic CeO2-mediated Sn0/Snδ+ redox cycle mechanism was proposed: oxygen vacancies generated on cerium oxides prompted water dissociation produce *OH *H species, where the former oxidize Sn0 into active Snδ+, facilitating key intermediate *OCHO help latter. This work may provide general design stable efficient catalysts for practical electrolyzers.

Язык: Английский

Surface Modification of 2D Photocatalysts for Solar Energy Conversion DOI Creative Commons
Chengyang Feng, Zhi‐Peng Wu, Kuo‐Wei Huang

и другие.

Advanced Materials, Год журнала: 2022, Номер 34(23)

Опубликована: Март 9, 2022

Abstract 2D materials show many particular properties, such as high surface‐to‐volume ratio, anisotropic degree, and adjustable chemical functionality. These unique properties in have sparked immense interest due to their applications photocatalytic systems, resulting significantly enhanced light capture, charge‐transfer kinetics, surface reaction. Herein, the research progress photocatalysts based on varied compositions functions, followed by specific modification strategies, is introduced. Fundamental principles focusing harvesting, charge separation, molecular adsorption/activation 2D‐material‐based system are systemically explored. The examples described here detail use of various energy‐conversion including water splitting, carbon dioxide reduction, nitrogen fixation, hydrogen peroxide production, organic synthesis. Finally, elaborating challenges possible solutions for developing these materials, review expected provide some inspiration future used efficient energy conversions.

Язык: Английский

Процитировано

337

Electrocatalytic CO2-to-C2+ with Ampere-Level Current on Heteroatom-Engineered Copper via Tuning *CO Intermediate Coverage DOI
Min Zheng, Pengtang Wang, Xing Zhi

и другие.

Journal of the American Chemical Society, Год журнала: 2022, Номер 144(32), С. 14936 - 14944

Опубликована: Авг. 4, 2022

An ampere-level current density of CO2 electrolysis is critical to realize the industrial production multicarbon (C2+) fuels. However, under such a large density, poor CO intermediate (*CO) coverage on catalyst surface induces competitive hydrogen evolution reaction, which hinders reduction reaction (CO2RR). Herein, we report reliable CO2-to-C2+ by heteroatom engineering Cu catalysts. The Cu-based compounds with (N, P, S, O) are electrochemically reduced heteroatom-derived significant structural reconstruction CO2RR conditions. It found that N-engineered (N-Cu) exhibits best productivity remarkable Faradaic efficiency 73.7% -1100 mA cm-2 and an energy 37.2% -900 cm-2. Particularly, it achieves C2+ partial -909 at -1.15 V versus reversible electrode, outperforms most reported In situ spectroscopy indicates adjusts *CO adsorption alters local H proton consumption in solution. Density functional theory studies confirm high strength N-Cu results from depressed HER promoted both bridge atop sites Cu, greatly reduces barrier for C-C coupling.

Язык: Английский

Процитировано

270

Porphyrin-based framework materials for energy conversion DOI Creative Commons

Jiawei Gu,

Yi Peng, Ting Zhou

и другие.

Deleted Journal, Год журнала: 2022, Номер 1, С. e9120009 - e9120009

Опубликована: Май 26, 2022

With the increasing demand for fuel causing serious environmental pollution, it is urgent to develop new and environmentally friendly energy conversion devices. These devices, however, require good, inexpensive materials electrodes so on. The multifunctional properties of porphyrins enable framework (e.g., metal-organic frameworks covalent organic frameworks) be applied in devices due their simple synthesis, high chemical stability, abundant metallic active sites, adjustable crystalline structure specific surface area. Herein, types porphyrin structural blocks are briefly reviewed. They can used as ligands or directly assembled with generate high-performance electro-/photo-catalysts. catalysts electro-/photo-catalytic water splitting, carbon dioxide reduction, electrocatalytic oxygen reduction also summarized introduced. At end article, we present challenges porphyrin-based above application corresponding solutions. We expect flourish coming years.

Язык: Английский

Процитировано

222

Dynamic Reconstitution Between Copper Single Atoms and Clusters for Electrocatalytic Urea Synthesis DOI
Xiaoxiao Wei, Yingying Liu, Xiaorong Zhu

и другие.

Advanced Materials, Год журнала: 2023, Номер 35(18)

Опубликована: Фев. 6, 2023

Electrocatalytic CN coupling between carbon dioxide and nitrate has emerged to meet the comprehensive demands of footprint closing, valorization waste, sustainable manufacture urea. However, identification catalytic active sites design efficient electrocatalysts remain a challenge. Herein, synthesis urea catalyzed by copper single atoms decorated on CeO2 support (denoted as Cu1 -CeO2 ) is reported. The catalyst exhibits an average yield rate 52.84 mmol h-1 gcat.-1 at -1.6 V versus reversible hydrogen electrode. Operando X-ray absorption spectra demonstrate reconstitution (Cu1 clusters (Cu4 during electrolysis. These electrochemically reconstituted Cu4 are real for electrocatalytic synthesis. Favorable reactions formation validated using operando synchrotron-radiation Fourier transform infrared spectroscopy theoretical calculations. Dynamic transformations single-atom configurations occur when applied potential switched open-circuit potential, endowing with superior structural electrochemical stabilities.

Язык: Английский

Процитировано

213

Cu-Zn-based alloy/oxide interfaces for enhanced electroreduction of CO2 to C2+ products DOI
Ziyang Zhang, Hao Tian, Lei Bian

и другие.

Journal of Energy Chemistry, Год журнала: 2023, Номер 83, С. 90 - 97

Опубликована: Май 11, 2023

Язык: Английский

Процитировано

148

Modulation of *CHxO Adsorption to Facilitate Electrocatalytic Reduction of CO2 to CH4 over Cu-Based Catalysts DOI
Jing Zhao, Peng Zhang,

Tenghui Yuan

и другие.

Journal of the American Chemical Society, Год журнала: 2023, Номер 145(12), С. 6622 - 6627

Опубликована: Март 20, 2023

Copper (Cu) can efficiently catalyze the electrochemical CO2 reduction reaction (CO2RR) to produce value-added fuels and chemicals, among which methane (CH4) has drawn attention due its high mass energy density. However, linear scaling relationship between adsorption energies of *CO *CHxO on Cu restricts selectivity toward CH4. Alloying a secondary metal in provides new freedom break relationship, thus regulating product distribution. This paper describes controllable electrodeposition approach alloying with oxophilic (M) steer pathway The optimized La5Cu95 electrocatalyst exhibits CH4 Faradaic efficiency 64.5%, partial current density 193.5 mA cm-2. introduction La could lower barrier for hydrogenation by strengthening M-O bond, would also promote breakage C-O bond *CH3O formation work avenue design Cu-based electrocatalysts achieve CO2RR through modulation behaviors key intermediates.

Язык: Английский

Процитировано

133

Stabilizing Copper by a Reconstruction-Resistant Atomic Cu–O–Si Interface for Electrochemical CO2 Reduction DOI
Xin Tan,

Kaian Sun,

Zewen Zhuang

и другие.

Journal of the American Chemical Society, Год журнала: 2023, Номер 145(15), С. 8656 - 8664

Опубликована: Апрель 8, 2023

Copper (Cu), a promising catalyst for electrochemical CO2 reduction (CO2R) to multi-electron products, suffers from an unavoidable and uncontrollable reconstruction process during the reaction, which not only may lead deactivation but also brings great challenges exploration of structure-performance relationship. Herein, we present efficient strategy stabilizing Cu with silica synthesize reconstruction-resistant CuSiOx amorphous nanotube catalysts abundant atomic Cu-O-Si interfacial sites. The strong interaction between makes sites ultrastable in CO2R reaction without any apparent reconstruction, thus exhibiting high CO2-to-CH4 selectivity (72.5%) stability (FECH4 remains above 60% after 12 h test). A remarkable conversion rate 0.22 μmol cm-2 s-1 was achieved flow cell device. This work provides very route design highly active stable Cu-based catalysts.

Язык: Английский

Процитировано

131

Carbon‐Confined Indium Oxides for Efficient Carbon Dioxide Reduction in a Solid‐State Electrolyte Flow Cell DOI

Zhitong Wang,

Yansong Zhou, Dongyu Liu

и другие.

Angewandte Chemie International Edition, Год журнала: 2022, Номер 61(21)

Опубликована: Март 8, 2022

Developing robust electrocatalysts and advanced devices is important for electrochemical carbon dioxide (CO2 ) reduction toward the generation of valuable chemicals. We present herein a carbon-confined indium oxide electrocatalyst stable efficient CO2 reduction. The reductive corrosion oxidative to metallic state during electrolysis could be prevented by protection, applied layer also optimizes reaction intermediate adsorption, which enables both high selectivity activity In liquid-phase flow cell, formate exceeds 90 % in wide potential window from -0.8 V -1.3 vs. RHE. continuous production ca. 0.12 M pure formic acid solution further demonstrated at current density 30 mA cm-2 solid-state electrolyte mediated reactor. This work provides significant concepts parallel development carbon-neutral technologies.

Язык: Английский

Процитировано

122

In Situ Reconstruction of Cu–N Coordinated MOFs to Generate Dispersive Cu/Cu2O Nanoclusters for Selective Electroreduction of CO2to C2H4 DOI
Chang Liu,

Xiang‐Da Zhang,

Jian-Mei Huang

и другие.

ACS Catalysis, Год журнала: 2022, Номер 12(24), С. 15230 - 15240

Опубликована: Ноя. 29, 2022

Electrochemical reduction of CO2 to obtain high-value-added feedstocks is a promising strategy alleviate the energy crisis. Cu-based catalysts generate multi-carbon products with high activity in reaction (CO2RR), although great challenges remain selectivity and stability catalysts. Here, highly active Cu/Cu2O nanoclusters were produced via situ electrochemical reconstruction using Cu–N coordinated MOFs as precursors for selective C2H4 synthesis, showing Faradaic efficiency 70.2 ± 1.7% toward partial current density 12.38 mA·cm–2 at −1.03 V vs RHE CO2RR. In infrared spectroscopy observation *CO*CO *CO*COH intermediates confirmed formation pathway, while Raman spectroscopy, ex XPS, HRTEM evidenced that coexisting Cu2O Cu sites. The method could be used synthesize electroreduction.

Язык: Английский

Процитировано

117

Electron‐Rich Bi Nanosheets Promote CO2 Formation for High‐Performance and pH‐Universal Electrocatalytic CO2 Reduction DOI

Zaiqi Li,

Bin Sun,

Difei Xiao

и другие.

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(11)

Опубликована: Янв. 20, 2023

Electrochemical CO2 reduction reaction (CO2 RR) to chemical fuels such as formate offers a promising pathway carbon-neutral future, but its practical application is largely inhibited by the lack of effective activation molecules and pH-universal feasibility. Here, we report an electronic structure manipulation strategy electron-rich Bi nanosheets, where electrons transfer from Cu donor acceptor in bimetallic Cu-Bi, enabling RR towards with concurrent high activity, selectivity stability (acidic, neutral alkaline) electrolytes. Combined situ Raman spectra computational calculations unravel that promotes ⋅- formation activate molecules, enhance adsorption strength *OCHO intermediate up-shifted p-band center, thus leading superior activity formate. Further integration robust nanosheets into III-V-based photovoltaic solar cell results unassisted artificial leaf solar-to-formate (STF) efficiency 13.7 %.

Язык: Английский

Процитировано

108