Identifying an Interfacial Stabilizer for Regeneration-Free 300 h Electrochemical CO2 Reduction to C2 Products DOI
Xinyu Wang,

Yawen Jiang,

Keke Mao

et al.

Journal of the American Chemical Society, Journal Year: 2022, Volume and Issue: 144(49), P. 22759 - 22766

Published: Dec. 1, 2022

The electrochemical CO2 reduction reaction (CO2RR) to produce high value-added hydrocarbons and oxygenates presents a sustainable compelling approach toward carbon-neutral society. However, uncontrollable migration of active sites during the CO2RR limits its catalytic ability simultaneously achieve C2 selectivity ultradurability. Here, we demonstrate that generated interfacial CuAlO2 species can efficiently stabilize highly over Cu-CuAlO2-Al2O3 catalyst under harsh conditions without regeneration for long-term test. We show this unique exhibits ultradurable performance with an 85% Faradaic efficiency 300 h Such simple engineering design unveiled in work would be adaptable develop various catalysts industrial-scale CO2RR.

Language: Английский

Anion-exchange membrane water electrolyzers and fuel cells DOI

Yaxiong Yang,

Peng Li, Xiaobo Zheng

et al.

Chemical Society Reviews, Journal Year: 2022, Volume and Issue: 51(23), P. 9620 - 9693

Published: Jan. 1, 2022

The key components, working management, and operating techniques of anion-exchange membrane water electrolyzers fuel cells are reviewed for the first time.

Language: Английский

Citations

252

Design strategies for markedly enhancing energy efficiency in the electrocatalytic CO2 reduction reaction DOI
Wenchuan Lai, Yan Qiao, Jiawei Zhang

et al.

Energy & Environmental Science, Journal Year: 2022, Volume and Issue: 15(9), P. 3603 - 3629

Published: Jan. 1, 2022

The review summarizes the recent strategies to improve energy efficiency of CO 2 electroreduction, a guiding metric for industrial application and economic feasibility, with emphasis on designing remarkable catalyst advanced electrolysis system.

Language: Английский

Citations

191

In‐Situ Constructuring of Copper‐Doped Bismuth Catalyst for Highly Efficient CO2 Electrolysis to Formate in Ampere‐Level DOI

Haidong Shen,

Yike Zhao,

Ling Zhang

et al.

Advanced Energy Materials, Journal Year: 2022, Volume and Issue: 13(1)

Published: Nov. 6, 2022

Abstract CO 2 electrochemical reduction (CO RR) can mitigate environmental issues while providing valuable products, yet challenging in activity, selectivity, and stability. Here, a CuS‐Bi S 3 heterojunction precursor is reported that situ reconstruct to Cu‐doped Bismuth (CDB) electrocatalyst during RR. The CDB exhibits an industrial‐compatible current density of −1.1 A cm −2 record‐high formate formation rate 21.0 mmol h −1 at −0.86 V versus the reversible hydrogen electrode toward RR formate, dramatically outperforming currently catalysts. Importantly, ultrawide potential region 1050 mV with high Faradaic efficiency over 90% superior long‐term stability for more than 100 −400 mA also be realized. Experimental theoretical studies reveal remarkable performance results from doping effect Cu which optimizes adsorption *OCHO boosts structural metallic bismuth catalyst. This study provides inspiration design element‐doping electrocatalysts enhance catalytic activity durability.

Language: Английский

Citations

81

Stability Issues in Electrochemical CO2 Reduction: Recent Advances in Fundamental Understanding and Design Strategies DOI Open Access
Wenchuan Lai, Yan Qiao, Yanan Wang

et al.

Advanced Materials, Journal Year: 2023, Volume and Issue: 35(51)

Published: Aug. 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.

Language: Английский

Citations

81

Applications of Metal–Organic Frameworks and Their Derivatives in Electrochemical CO2 Reduction DOI Creative Commons
Chengbo Li,

Yuan Ji,

Youpeng Wang

et al.

Nano-Micro Letters, Journal Year: 2023, Volume and Issue: 15(1)

Published: April 30, 2023

Abstract Electrochemically reducing CO 2 to more reduced chemical species is a promising way that not only enables the conversion of intermittent energy resources stable fuels, but also helps build closed-loop anthropogenic carbon cycle. Among various electrocatalysts for electrochemical reduction, multifunctional metal–organic frameworks (MOFs) have been employed as highly efficient and selective heterogeneous due their ultrahigh porosity topologically diverse structures. Up now, great progress has achieved in design synthesis active MOF-related catalysts reduction reaction (CO RR), corresponding mechanisms thoroughly studied. In this review, we summarize recent applying MOFs derivatives RR, with focus on strategies electrolyzers. We first discussed different RR products introduced commonly applied electrolyzer configurations current system. Then, an overview several categories (CO, HCOOH, CH 4 , 3 OH, multi-carbon chemicals) generated from or via was discussed. Finally, offer some insights perspectives future development reduction. aim provide new into field further guide research large-scale applications.

Language: Английский

Citations

78

In Situ Structural Reconstruction to Generate the Active Sites for CO2 Electroreduction on Bismuth Ultrathin Nanosheets DOI
Yuliang Yuan, Qiyou Wang, Yan Qiao

et al.

Advanced Energy Materials, Journal Year: 2022, Volume and Issue: 12(29)

Published: June 16, 2022

Abstract Electrochemical structural reconstruction of catalysts may generate real active sites that differ from the initial catalyst, but is often ignored. Herein, combining in situ and ex techniques, it identified bismuth nanosheets (NS) dotted with large numbers coordinatively unsaturated pit produced via Bi(OH) 3 NS. Such reconstructed Bi NS shows greatly improved catalytic activity toward CO 2 electroreduction, a 2.6‐fold increase current density compared intact NS, high Faradaic efficiency for HCOO − production (>95%), an extraordinary turnover frequency 0.35 s −1 at −0.98 V RHE . In addition, delivers industrial‐relevant 325 mA cm −2 without compromising selectivity flow cell. The mechanistic studies demonstrate these acting as favor stabilization key intermediate *OCHO, which thus facilitate reaction kinetics production. This work not only provides unique perspective on construction efficient also implies importance recognition reconstruction.

Language: Английский

Citations

74

Nanograin-Boundary-Abundant Cu2O-Cu Nanocubes with High C2+ Selectivity and Good Stability during Electrochemical CO2 Reduction at a Current Density of 500 mA/cm2 DOI
Qiqi Wu, Ruian Du, Peng Wang

et al.

ACS Nano, Journal Year: 2023, Volume and Issue: 17(13), P. 12884 - 12894

Published: June 20, 2023

Surface and interface engineering, especially the creation of abundant Cu0/Cu+ interfaces nanograin boundaries, is known to facilitate C2+ production during electrochemical CO2 reductions over copper-based catalysts. However, precisely controlling favorable boundaries with surface structures (e.g., Cu(100) facets Cu[n(100)×(110)] step sites) simultaneously stabilizing challenging, since Cu+ species are highly susceptible be reduced into bulk metallic Cu at high current densities. Thus, an in-depth understanding structure evolution Cu-based catalysts under realistic CO2RR conditions imperative, including formation stabilization interfaces. Herein we demonstrate that well-controlled thermal reduction Cu2O nanocubes a CO atmosphere yields remarkably stable Cu2O-Cu nanocube hybrid catalyst (Cu2O(CO)) possessing density interfaces, facets, sites. The Cu2O(CO) electrocatalyst delivered Faradaic efficiency 77.4% (56.6% for ethylene) industrial 500 mA/cm2. Spectroscopic characterizations morphological studies, together in situ time-resolved attenuated total reflection-surface enhanced infrared absorption spectroscopy (ATR-SEIRAS) established morphology interfacial sites as-prepared were preserved polarization densities due nanograin-boundary-abundant structure. Furthermore, on acted increase *CO adsorption density, thereby increasing opportunity C-C coupling reactions, leading selectivity.

Language: Английский

Citations

71

From Single Crystal to Single Atom Catalysts: Structural Factors Influencing the Performance of Metal Catalysts for CO2 Electroreduction DOI
Cedric David Koolen, Wen Luo, Andreas Züttel

et al.

ACS Catalysis, Journal Year: 2022, Volume and Issue: 13(2), P. 948 - 973

Published: Dec. 30, 2022

With the electrochemical CO2 reduction reaction (CO2RR), can be used as a feedstock to produce value-added chemicals and fuels while storing renewable energy. For its enormous potential, an extensive research effort has been launched find most active electrocatalyst. The of catalyst size tested proven key approach increase activity CO2RR reducing capital cost. However, catalytic selectivity is not linearly related due influence many other structural factors. Thus, in-depth knowledge structure-performance relationships metal catalysts with different sizes aids in designing efficient electrocatalysts for CO2RR. This Review surveys three decades on categorizes various into four regimes, namely, bulk materials form single crystals, nanoparticles, clusters, single-atom catalysts. effects factors, including crystal facet, coordination environment, metal–support interactions, etc., each regime are discussed. Finally, general conclusions provided perspectives future directions better understanding further development selective

Language: Английский

Citations

70

Spatially and temporally understanding dynamic solid–electrolyte interfaces in carbon dioxide electroreduction DOI
Jiali Wang,

Hui‐Ying Tan,

Ming–Yu Qi

et al.

Chemical Society Reviews, Journal Year: 2023, Volume and Issue: 52(15), P. 5013 - 5050

Published: Jan. 1, 2023

The ubiquity of solid-liquid interfaces in nature and the significant role their atomic-scale structure determining interfacial properties have led to intensive research. Particularly electrocatalysis, however, a molecular-level picture that clearly describes dynamic structures organizations with correlation preferred reaction pathways electrochemical reactions remains poorly understood. In this review, CO2 electroreduction (CO2RR) is spatially temporally understood as result intricate interactions at interface, which features are highly relevant. We start discussion current understandings model development associated charged interface well its landscape. further highlight interactive dynamics from field, catalyst surface charges various gradients electrolyte water under CO2RR working conditions, emphasis on interfacial-structure dependence catalytic reactivity/selectivity. Significantly, probing energy-dependent "in situ characterization map" for based complementary situ/operando techniques proposed, aiming present comprehensive electrocatalysis provide more unified research framework. Moreover, recent milestones both experimental theoretical aspects establish correct profile stressed. Finally, we key scientific challenges related perspectives toward future opportunities exciting frontier.

Language: Английский

Citations

68

Selective production of ethylene glycol at high rate via cascade catalysis DOI
Lei Fan, Yilin Zhao, Lei Chen

et al.

Nature Catalysis, Journal Year: 2023, Volume and Issue: 6(7), P. 585 - 595

Published: June 26, 2023

Language: Английский

Citations

67