Electrochemical reduction of carbon dioxide to multicarbon (C₂₊) products: challenges and perspectives

Energy & Environmental Science, Год журнала: 2023, Номер 16(11), С. 4714 - 4758

Опубликована: Янв. 1, 2023

This review analyzes advanced catalysts and C 2+ synthesis mechanisms based on theoretical explorations in situ / operando characterizations. Triphasic interface optimization is discussed for the potential of industry-compatible stability.

Язык: Английский

---

CO2 electroreduction to multicarbon products in strongly acidic electrolyte via synergistically modulating the local microenvironment

Nature Communications, Год журнала: 2022, Номер 13(1)

Опубликована: Дек. 9, 2022

Electrochemical CO2 reduction to multicarbon products faces challenges of unsatisfactory selectivity, productivity, and long-term stability. Herein, we demonstrate electroreduction in strongly acidic electrolyte (pH ≤ 1) on electrochemically reduced porous Cu nanosheets by combining the confinement effect cation synergistically modulate local microenvironment. A Faradaic efficiency 83.7 ± 1.4% partial current density 0.56 0.02 cm-2, single-pass carbon 54.4%, stable electrolysis 30 h a flow cell are demonstrated for aqueous consisting sulfuric acid KCl with pH 1. Mechanistically, accumulated species (e.g., K+ OH-) Helmholtz plane account selectivity activity toward kinetically reducing proton coverage thermodynamically favoring conversion. We find that cations facilitate C-C coupling through interaction between key intermediate *OCCO.

Язык: Английский

---

Recent advances on electrocatalytic CO2 reduction to resources: Target products, reaction pathways and typical catalysts

Chemical Engineering Journal, Год журнала: 2022, Номер 453, С. 139663 - 139663

Опубликована: Окт. 8, 2022

Язык: Английский

---

Turning Waste into Wealth: Sustainable Production of High-Value-Added Chemicals from Catalytic Coupling of Carbon Dioxide and Nitrogenous Small Molecules

ACS Nano, Год журнала: 2022, Номер 16(11), С. 17911 - 17930

Опубликована: Окт. 31, 2022

Carbon neutrality is one of the central topics not only scientific community but also majority human society. The development highly efficient carbon dioxide (CO2) capture and utilization (CCU) techniques expected to stimulate routes concepts go beyond fossil fuels provide more economic benefits for a carbon-neutral economy. While various single-carbon (C1) multi-carbon (C2+) products have been selectively produced date, scope CCU can be further expanded valuable chemicals simple species by integration nitrogenous reactants into CO2 reduction. In this Review, research progress toward sustainable production high-value-added (urea, methylamine, ethylamine, formamide, acetamide, glycine) from catalytic coupling small molecules (NH3, N2, NO3–, NO2–) highlighted. C–N bond formation key mechanistic step in N-integrated reduction, so we focus on possible pathways starting reduction processes as well attributes that enable coupling. We propose directions prospects field, aiming inspire future investigations achieve comprehensive improvement performance product systems.

Язык: Английский

---

Understanding and leveraging the effect of cations in the electrical double layer for electrochemical CO2 reduction

Chem Catalysis, Год журнала: 2022, Номер 2(6), С. 1267 - 1276

Опубликована: Апрель 18, 2022

Язык: Английский

---

Rare‐Earth Single‐Atom Catalysts: A New Frontier in Photo/Electrocatalysis

Small Methods, Год журнала: 2022, Номер 6(8)

Опубликована: Июнь 25, 2022

Abstract Single‐atom catalysts (SACs) provide well‐defined active sites with 100% atom utilization, and can be prepared using a wide range of support materials. Therefore, they are attracting global attention, especially in the fields energy conversion storage. To date, research has focused on transition‐metal precious‐metal‐based SACs. More recently, rare‐earth (RE)‐based SACs have emerged as new frontier photo/electrocatalysis owing to their unique electronic structure arising from spin‐orbit coupling 4f valence orbitals, unsaturated coordination environment, behavior charge‐transport bridges. However, systematic review role RE sites, catalytic mechanisms, synthetic methods for is lacking. this review, latest developments having applications summarized discussed. First, theoretical advantages briefly introduced, focusing roles orbitals coupled levels. In addition, most recent progress several important photo/electrocatalytic reactions corresponding mechanisms Further, strategies production reported. Finally, challenges development highlighted, along future directions perspectives.

Язык: Английский

---

In-situ/operando Raman techniques for in-depth understanding on electrocatalysis

Chemical Engineering Journal, Год журнала: 2023, Номер 461, С. 141939 - 141939

Опубликована: Фев. 16, 2023

Язык: Английский

---

Stability Issues in Electrochemical CO₂ Reduction: Recent Advances in Fundamental Understanding and Design Strategies

Advanced Materials, Год журнала: 2023, Номер 35(51)

Опубликована: Авг. 11, 2023

Electrochemical CO2 reduction reaction (CO2 RR) offers a promising approach to close the anthropogenic carbon cycle and store intermittent renewable energy in fuels or chemicals. On path commercializing this technology, achieving long-term operation stability is central requirement but still confronts challenges. This motivates organize present review systematically discuss issue of RR. starts from fundamental understanding on destabilization mechanisms RR, with focus degradation electrocatalyst change microenvironment during continuous electrolysis. Subsequently, recent efforts catalyst design stabilize active sites are summarized, where increasing atomic binding strength resist surface reconstruction highlighted. Next, optimization electrolysis system enhance by maintaining especially mitigating flooding carbonate problems demonstrated. The manipulation conditions also enables prolong RR lifespan through recovering catalytically mass transport process. finally ends up indicating challenges future opportunities.

Язык: Английский

---

Local reaction environment in electrocatalysis

Chemical Society Reviews, Год журнала: 2024, Номер 53(4), С. 2022 - 2055

Опубликована: Янв. 1, 2024

Beyond conventional electrocatalyst engineering, recent studies have unveiled the effectiveness of manipulating local reaction environment in enhancing performance electrocatalytic reactions. The general principles and strategies environmental engineering for different processes been extensively investigated. This review provides a critical appraisal advancements aiming to comprehensively assess this emerging field. It presents interactions among surface structure, ions distribution electric field relation environment. Useful protocols such as interfacial reactant concentration, mass transport rate, adsorption/desorption behaviors, binding energy are in-depth discussed toward modifying Meanwhile, electrode physical structures cell configurations viable optimization methods environments. In combination with

Язык: Английский

---

Tailoring the Catalytic Microenvironment of Cu₂O with SiO₂ to Enhance C₂₊ Product Selectivity in CO₂ Electroreduction

ACS Catalysis, Год журнала: 2023, Номер 13(7), С. 4444 - 4453

Опубликована: Март 18, 2023

Achieving high activity and selectivity of multicarbon products in the CO2 reduction reaction (CO2RR) on Cu-based electrocatalysts remains challenging due to limited concentration local OH–, sluggish diffusion, competitive hydrogen evolution reaction. Herein, we report aerophilic nanocomposites hydrophobic SiO2 aerosol Cu2O nanocubes tailor microenvironment for enhancing electroreduction 0.1 M KHCO3 aqueous electrolyte. Combined situ infrared analysis, molecular dynamics simulations, density functional theory calculations reveal that composite Cu2O/SiO2 enriches hydroxyl by blocking between OH– HCO3–, accelerates diffusion coefficient (from 2.67 × 10–10 8.46 m2 s–1), renders a lower dissociation energy H2O than bicarbonate (0.49 vs 1.24 eV (111)) as compared neat Cu2O. Consequently, promotes formation C2+ (Faradaic efficiency FEC2+ from 52.4 75.6%) suppresses generation (FEH2 30.0 9.6%) at −1.2 V versus reversible electrode. The results provide insight into improvement CO2RR electrocatalysis regulating alkalinity, transportation, permeability.

Язык: Английский

---