Review on strategies for improving the added value and expanding the scope of CO₂ electroreduction products

Chemical Society Reviews, Journal Year: 2024, Volume and Issue: 53(10), P. 5149 - 5189

Published: Jan. 1, 2024

This review summarizes promising strategies including the design of catalysts and construction coupled electrocatalytic reaction systems, aimed at achieving selective production various products from CO 2 electroreduction.

Language: Английский

---

Unveiling pH‐Dependent Adsorption Strength of *CO₂⁻ Intermediate over High‐Density Sn Single Atom Catalyst for Acidic CO₂‐to‐HCOOH Electroreduction

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(14)

Published: Feb. 16, 2024

Abstract The acidic electrochemical CO 2 reduction reaction (CO RR) for direct formic acid (HCOOH) production holds promise in meeting the carbon‐neutral target, yet its performance is hindered by competing hydrogen evolution (HER). Understanding adsorption strength of key intermediates electrolyte indispensable to favor RR over HER. In this work, high‐density Sn single atom catalysts (SACs) were prepared and used as catalyst, reveal pH‐dependent coverage *CO − intermediatethat enables enhanced towards HCOOH production. At pH=3, SACs could deliver a high Faradaic efficiency (90.8 %) formation corresponding partial current density up −178.5 mA cm −2 . detailed situ attenuated total reflection Fourier transform infrared (ATR‐FTIR) spectroscopic studies that favorable alkaline microenvironment formed near surface SACs, even electrolyte. More importantly, intermediate unravelled which turn affects competition between HER

Language: Английский

---

Beyond Leverage in Activity and Stability toward CO₂ Electroreduction to Formate over a Bismuth Catalyst

ACS Catalysis, Journal Year: 2024, Volume and Issue: 14(10), P. 8050 - 8061

Published: May 8, 2024

The direct production of formate from CO2 over Bi-based catalysts offers a promising route for producing important chemicals using renewable electricity. Nevertheless, limited by the unstable structure and states under electrochemical conditions, electroreduction to is still facing trade-off between activity stability, especially at high current densities. Herein, we reported metal–carbon interfacial modulation strategy synthesize cross-linked defective carbon-modified Bi nanoparticle (Bi-DC) catalyst with stable spatial unique CO2-philic hydrophobic interface. As result, Bi-DC featured remarkable ability in near neutral electrolyte (1 M KHCO3) was even comparable CO2-to-formate strongly basic systems, along partial density formation rate −378 mA cm–2 7 mmol h–1, respectively. Also, it achieved electrolysis 120 h 0.4 A membrane electrode assembly reactor operated stably an industrial large 5 A. carbon species promoted reconstruction dispersion active component Bi, together confinement effect that facilitated long-term electrolysis.

Language: Английский

---

pH‐Universal Electrocatalytic CO₂ Reduction with Ampere‐Level Current Density on Doping‐Engineered Bismuth Sulfide

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(32)

Published: May 27, 2024

Abstract The practical application of the electrocatalytic CO 2 reduction reaction (CO RR) to form formic acid fuel is hindered by limited activation molecules and lack universal feasibility across different pH levels. Herein, we report a doping‐engineered bismuth sulfide pre‐catalyst (BiS‐1) that S partially retained after electrochemical reconstruction into metallic Bi for RR formate/formic with ultrahigh performance wide range. best BiS‐1 maintains Faraday efficiency (FE) ~95 % at 2000 mA cm −2 in flow cell under neutral alkaline solutions. Furthermore, catalyst shows unprecedentedly high FE (~95 %) current densities from 100 1300 acidic Notably, density can reach 700 while maintaining above 90 membrane electrode assembly electrolyzer operate stably 150 h 200 . In situ spectra functional theory calculations reveals doping modulates electronic structure effectively promotes formation HCOO* intermediate generation. This work develops efficient stable electrocatalysts sustainable production.

Language: Английский

---

Ultra‐Fast Pulsed Discharge Preparation of Coordinatively Unsaturated Asymmetric Copper Single‐Atom Catalysts for CO₂ Reduction

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: 34(16)

Published: Jan. 3, 2024

Abstract Single‐atom catalysts possess great potential for applications in electrochemical carbon dioxide reduction reactions. Recently, the fast and low‐cost preparation of highly efficient single‐atom remains a challenge. Herein, high‐density current generated by pulsed discharge is employed formation graphene aerogel anchored Cu single atom perfectly. The atoms decomposed Cu(NO 3 ) 2 •xH O are fixed on under local transient high temperature intense electromagnetic field. activity selectivity formic acid correlated with coordinatively unsaturated Cu─N 1 moieties, reaching an optimal Faradaic efficiency (93.7%) at −0.9 V versus reversible hydrogen electrode (RHE). In situ characterizations reveal that asymmetric Cu─N/O structure pinched state displays better catalytic CO RR. Density functional theory results indicate sites regulate adsorption configuration intermediates lower energy barrier hydrogenation * OCHO species, thereby promoting ‐to‐HCOOH conversion.

Language: Английский

---

Reconstructed Bismuth Oxide through in situ Carbonation by Carbonate‐containing Electrolyte for Highly Active Electrocatalytic CO₂ Reduction to Formate

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 63(9)

Published: Dec. 26, 2023

The catalyst-reconstruction makes it challenging to clarify the practical active sites and unveil actual reaction mechanism during CO

Language: Английский

---

High C‐Selectivity for Urea Synthesis Through O‐Philic Adsorption to Form *OCO Intermediate on Ti‐MOF Based Electrocatalysts

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: 34(34)

Published: March 12, 2024

Abstract The advent of utilizing nitrate (NO 3 − ) for electrochemical co‐reduction with carbon dioxide (CO 2 to effectively synthesize high‐value‐added organic nitrogen compounds has captured the attention environmental and energy fields. C─N coupling is a key step during process. An effective strategy improve efficiency synthesis explore optimal reaction pathway active species. Herein, p‐type semiconductor nanosphere (Ti‐DHTP) presented urea by combining CO NO . At low voltage −0.6 V versus RHE, exhibits 95.5% C‐selectivity 21.75% Faraday efficiency. Comparative experiments, in situ theoretical simulations confirm that new from * NH OCO intermediates become Ti‐DHTP‐driven coupling. Moreover, more efficient intermediate inhibits generation large amounts C‐bearing by‐products. Meanwhile, Ti‐DHTP difficulty hydrogenating form COOH reduction leading subsequent inability produce intermediates. This work reveals mechanism, which provides feasible future research on nitrogen‐bearing compounds.

Language: Английский

---

Low-temperature microwave-assisted synthesis of Bi2WO6/Bi2S3 heterojunction for photocatalytic reduction of Cr(VI) in industrial wastewater

Journal of Alloys and Compounds, Journal Year: 2024, Volume and Issue: 997, P. 174842 - 174842

Published: May 14, 2024

Language: Английский

---

Enhancing Electrocatalytic Water Oxidation of NiFe-LDH Nanosheets via Bismuth-Induced Electronic Structure Engineering

ACS Applied Materials & Interfaces, Journal Year: 2023, Volume and Issue: 15(50), P. 58784 - 58793

Published: Dec. 12, 2023

The design and synthesis of high-efficiency electrocatalysts are great practical significance in electrocatalytic water splitting, specifically accelerating the slow oxygen evolution reaction (OER). Herein, a self-supported bismuth-doped NiFe layered double hydroxide (LDH) nanosheet array for splitting was successfully constructed on nickel foam by one-step hydrothermal strategy. Benefiting from abundant active sites two-dimensional nanosheets electronic effect Bi-doped LDH, optimal Bi0.2NiFe LDH electrocatalyst exhibits excellent OER performance basic media. It only requires an overpotential 255 mV to drive 50 mA cm–2 low Tafel slope 57.49 dec–1. calculation density functional theory (DFT) further shows that incorporation Bi into could obviously overcome step H2O adsorption during progress. This work provides simple effective strategy improving LDHs, which is significance.

Language: Английский

---

Promoting Electrochemical CO₂ Reduction to Formate via Sulfur‐Assisted Electrolysis

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: unknown

Published: May 16, 2024

Abstract Electrochemical CO 2 reduction reaction (CO RR) provides a renewable approach to transform produce chemicals and fuels. Unfortunately, it faces the challenges of sluggish activation slow water dissociation. This study reports modification Bi‐based electrocatalyst by S, which leads remarkable enhancement in activity selectivity during electrochemical formate. Based on comprehensive situ examinations kinetic evaluations, is observed that presence S species over Bi catalyst can significantly enhance its interaction with K + (H O) n , facilitating fast dissociation molecules generate protons. Further attenuated total reflectance surface‐enhanced infrared absorption spectroscopy (ATR‐SEIRAS) Raman measurements reveal able decrease oxidation state active site, effectively facilitate HCOO * intermediate formation while suppressing competing hydrogen evolution reaction. Consequently, S‐modified achieves impressive RR performance, reaching formate Faradaic efficiency (FE ) 91.2% at partial current density ≈135 mA cm −2 potential −0.8 V versus RHE an alkaline electrolyte.

Language: Английский

---