Electroreduction of CO₂: Advances in the Continuous Production of Formic Acid and Formate

ACS Energy Letters, Год журнала: 2023, Номер 8(4), С. 1992 - 2024

Опубликована: Март 30, 2023

The study of the electrochemical CO2 reduction to obtain formate (HCOO–) or formic acid (HCOOH) is receiving much attention as a promising technology. Since continuous–mode operation has become necessary for practical implementation reduction, recent years have seen rapid increase in number research approaches focusing on this aspect. This Focus Review provides unified discussion available studies continuous electroreduction HCOO–/HCOOH, considering different important features process design. Moreover, paper quantitatively assesses performance that involve reactors converting HCOOH/HCOO–, comparing relevant typically used figures merit, including energy consumption. Although some trade-offs already been achieved, simultaneous optimization all merit remains challenge. Finally, concluding remarks highlight detected trends and discuss aspects will be tackled by future field.

Язык: Английский

---

Electrocatalytic Waste-Treating-Waste Strategy for Concurrently Upgrading of Polyethylene Terephthalate Plastic and CO₂ into Value-Added Formic Acid

ACS Catalysis, Год журнала: 2023, Номер 13(21), С. 14163 - 14172

Опубликована: Окт. 20, 2023

Polyethylene terephthalate (PET) plastic and CO2 pollution have seriously threatened the ecological environment caused a huge waste of carbon resources. Herein, we report an electrocatalytic waste-treating-waste strategy for concurrently upgrading PET wastes into value-added formic acid (HCOOH), in which both anode (oxygen-vacancy-rich Ni(OH)2-VO) cathode (Bi/Bi2O3 heterostructure) electrocatalysts were elaborately designed from derivatives. Impressively, as-prepared Ni(OH)2-VO Bi/Bi2O3 achieve high selectivity HCOOH (86 91%, respectively) with industrial-level current densities at ultralow potentials (300 mA cm–2 1.6 V −272 −1.4 V, respectively). Further experimental theoretical results reveal that abundant oxygen vacancies will largely facilitate formation Ni3+ species accelerate subsequent processes dehydrogenation C–C bond breakage during upcycling. Meanwhile, interface electron transfer Bi2O3 to Bi benefits keeping valence sites optimizes adsorption OCHO* intermediate, thereby endowing efficient performance toward reduction HCOOH. As proof concept, solar-powered flow reactor real-time monitoring control functions was designed, realized record Faradaic efficiency 181% This work offers opportunities utilization provides constructive guidance design advanced converting valuable chemicals.

Язык: Английский

---

Atomically Dispersed W₁–O₃ Bonded on Pd Metallene for Cascade NO Electroreduction to NH₃

ACS Catalysis, Год журнала: 2023, Номер 13(14), С. 9550 - 9557

Опубликована: Июль 5, 2023

Electrocatalytic NO reduction to NH3 (NORR) offers a prospective method for removing hazardous and producing valuable simultaneously. Herein, we demonstrate that atomically dispersed W on Pd metallene (W1Pd) can be an efficient robust NORR catalyst. Atomic coordination characterizations unravel single atoms exist as W1–O3 moieties bonded metallene. In situ spectroscopic measurements theoretical calculations reveal the synergistic cascade effect of promote energetics W1Pd, in which activation hydrogenation occur W1–O3, while dissociates H2O donates protons required NH3. Consequently, W1Pd exhibits yield rate 758.5 μmol h–1 cm–2 with NH3-Faradaic efficiency 91.3% flow cell (272.1 93.7% H-type cells), ranking almost highest performance among all reported catalysts.

Язык: Английский

---

Enhanced Electrochemical CO₂ Reduction to Formate over Phosphate‐Modified In: Water Activation and Active Site Tuning

Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(27)

Опубликована: Апрель 26, 2024

Electrochemical CO

Язык: Английский

---

Modulation of the electronic structure of metallic bismuth catalysts by cerium doping to facilitate electrocatalytic CO₂ reduction to formate

Journal of Materials Chemistry A, Год журнала: 2024, Номер 12(13), С. 7528 - 7535

Опубликована: Янв. 1, 2024

Bi(0) metal was utilized as a CO 2 RR catalyst to achieve enhanced durability in cathodic applications. Besides, the activity effectively improved by promising strategy of electronic structure modulation through Ce doping.

Язык: Английский

---

MOF-Based Electrocatalysts: An Overview from the Perspective of Structural Design

Chemical Reviews, Год журнала: 2025, Номер unknown

Опубликована: Фев. 18, 2025

The electrocatalytic technique, as an efficient energy storage and conversion technology, has attracted significant attention to address exhaustion environmental pollution. Usually, the activity selectivity of reactions are largely dominated by dynamic process occurring on electrocatalysts. Therefore, high-performance electrocatalysts, which can dominate pathway barrier reactions, great significance for advancement technique. Metal-organic frameworks (MOFs), emerging crystalline porous materials, present structural component advantages including well-defined structure, high surface area, large porosity, diverse components, easy tailorability, demonstrating fantastic potential precise fabrication In this Review, strategies in electrocatalysts based MOF-related materials specifically introduced from aspects catalytic site design microenvironment modulation around sites. Furthermore, representative progress achieved various applications employing MOF-based is systematically summarized, with special emphasis MOFs performance optimization. Finally, remaining challenges future perspectives further highlighted.

Язык: Английский

---

Anion Exchange Facilitates the In Situ Construction of Bi/BiO Interfaces for Enhanced Electrochemical CO₂‐to‐Formate Conversion Over a Wide Potential Window

Small, Год журнала: 2023, Номер 19(43)

Опубликована: Июнь 27, 2023

Electrochemical reduction of CO2 (CO2 RR) into value-added products is a promising strategy to reduce energy consumption and solve environmental issues. Formic acid/formate one the high-value, easy-to-collect, economically viable products. Herein, reconstructed Bi2 O2 CO3 nanosheets (BOCR NSs) are synthesized by an in situ electrochemical anion exchange from SO4 as pre-catalyst. The BOCR NSs achieve high formate Faradaic efficiency (FEformate ) 95.7% at -1.1 V versus reversible hydrogen electrode (vs. RHE), maintain FEformate above 90% wide potential range -0.8 -1.5 H-cell. spectroscopic studies reveal that obtained undergo further promote self-reduction metallic Bi construct Bi/BiO active site facilitate formation OCHO* intermediate. This result demonstrates can be used rational design performance catalysts toward RR.

Язык: Английский

---

Metal‐Organic Framework (MOF)‐Based Clean Energy Conversion: Recent Advances in Unlocking its Underlying Mechanisms

Small, Год журнала: 2023, Номер 20(20)

Опубликована: Дек. 21, 2023

Abstract Carbon neutrality is an important goal for humanity . As eco‐friendly technology, electrocatalytic clean energy conversion technology has emerged in the 21st century. Currently, metal‐organic framework (MOF)‐based electrocatalysis, including oxygen reduction reaction (ORR), evolution (OER), hydrogen (HER), oxidation (HOR), carbon dioxide (CO 2 RR), nitrogen (NRR), are mainstream catalytic reactions, which driven by electrocatalysis. In this paper, current advanced characterizations analyses of MOF‐based reactions have been described details, such as density function theory (DFT), machine learning, operando/in situ characterization, provide in‐depth mechanisms related to above reported past years. The practical applications that developed some responses application values, fuel cells, metal‐air batteries, and water splitting also demonstrated. This paper aims maximize potential electrocatalysts field catalysis, shed light on development intense situations.

Язык: Английский

---

Enriching Metal–Oxygen Species and Phosphate Modulating of Active Sites for Robust Electrocatalytical CO₂ Reduction

Advanced Materials, Год журнала: 2023, Номер 35(46)

Опубликована: Июль 24, 2023

Direct electrochemical reduction of CO2 (CO2 RR) into value-added chemicals is a promising solution to reduce carbon emissions. The activity RR influenced deeply by the reaction microenvironment and electronic properties catalysts. Herein, surface PO43- anions are tuned modulate local indium-based catalyst with abundant metal-oxygen species enabling efficient conversion HCOO- . Indium nanoparticles coupled (PO43- -In NPs) achieve high selectivity up 91.4% at low potential -0.98 V versus reversible hydrogen electrode (versus RHE) partial current density 279.3 mA cm-2 -1.1 RHE in flow cell. In situ ex characterizations confirm keep stable on indium during RR, accelerating generation OCHO* intermediate. From functional theory calculations, enrich substrate optimize structure catalysts induce massive K+ ions interface, thus reducing activation energy barrier RR.

Язык: Английский

---

A comparative study on carbon neutral hydrogen carrier production: Formic acid from CO2 vs. ammonia

Journal of CO2 Utilization, Год журнала: 2024, Номер 82, С. 102756 - 102756

Опубликована: Апрель 1, 2024

Hydrogen (H2) is increasingly recognized as a key player in the journey towards carbon neutrality, with ammonia (NH3) and formic acid (FA) emerging significant hydrogen vectors. This review highlights advancements catalyst efficiency for FA synthesis from CO2, particularly bismuth (Bi) tin (Sn) catalysts. It investigates diverse NH3 production methodologies, such electrochemical, thermochemical, photochemical processes, underscores integration of renewables to address their energy demands. The study also reviews novel materials like metal-organic frameworks (MOFs) carbon-based catalysts that could enhance catalytic effectiveness. Transitioning lab-scale models industrial-scale applications requires addressing longevity process enhancement, it suggests investigating hybrid systems might offer improved yields. Concluding directive future research, advocates scalable, economically viable, environmentally sustainable CO2 conversion technologies, underscoring essential roles reduced emissions.

Язык: Английский

---