Acidic CO2 Electrolysis Addressing the “Alkalinity Issue” and Achieving High CO2 Utilization DOI
Ting Zhang,

Jinlei Zhou,

Ting Luo

et al.

Chemistry - A European Journal, Journal Year: 2023, Volume and Issue: 29(46)

Published: June 7, 2023

Abstract Electrochemical CO 2 reduction reaction (CO RR) provides a promising approach for sustainable chemical fuel production of carbon neutrality. Neutral and alkaline electrolytes are predominantly employed in the current electrolysis system, but with striking drawbacks (bi)carbonate 3 2− /HCO − ) formation crossover due to rapid thermodynamically favourable between hydroxide (OH , resulting low utilization efficiency short‐lived catalysis. Very recently, RR acidic media can effectively address issue; however, competing hydrogen evolution (HER) is more kinetically electrolytes, which dramatically reduces conversion efficiency. Thus, it big challenge suppress HER accelerate RR. In this review, we begin by summarizing recent progress electrolysis, discussing key factors limiting application electrolytes. We then systematically discuss addressing strategies including electrolyte microenvironment modulation, alkali cations adjusting, surface/interface functionalization, nanoconfinement structural design, novel electrolyzer exploitation. Finally, new challenges perspectives suggested. believe timely review arouse researchers′ attention crossover, inspire insights solve “alkalinity problem” enable as technology.

Language: Английский

Challenges and Opportunities in Electrocatalytic CO2 Reduction to Chemicals and Fuels DOI Creative Commons
Xiaojie She, Yifei Wang, Hui Xu

et al.

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 61(49)

Published: Aug. 22, 2022

The global temperature increase must be limited to below 1.5 °C alleviate the worst effects of climate change. Electrocatalytic CO

Language: Английский

Citations

157
Heterogeneous Catalysis for CO2 Conversion into Chemicals and Fuels DOI Creative Commons
Dunfeng Gao, Wanjun Li, Hanyu Wang

et al.

Transactions of Tianjin University, Journal Year: 2022, Volume and Issue: 28(4), P. 245 - 264

Published: Aug. 1, 2022

Abstract Catalytic conversion of CO 2 into chemicals and fuels is a viable method to reduce carbon emissions achieve neutrality. Through thermal catalysis, electrocatalysis, photo(electro)catalysis, can be converted wide range valuable products, including CO, formic acid, methanol, methane, ethanol, acetic propanol, light olefins, aromatics, gasoline, as well fine chemicals. In this mini-review, we summarize the recent progress in heterogeneous catalysis for highlight some representative studies different routes. The structure–performance correlations typical catalytic materials used reactions have been revealed by combining advanced situ/operando spectroscopy microscopy characterizations density functional theory calculations. selectivity toward single reduction product/fraction should further improved at an industrially relevant rate with considerable stability future. Graphical

Language: Английский

Citations

87
Pure-water-fed, electrocatalytic CO2 reduction to ethylene beyond 1,000 h stability at 10 A DOI Creative Commons
Xiaojie She,

Ling-Ling Zhai,

Yifei Wang

et al.

Nature Energy, Journal Year: 2024, Volume and Issue: 9(1), P. 81 - 91

Published: Jan. 5, 2024

Abstract Electrocatalytic CO 2 reduction at near-ambient temperatures requires a complex inventory of protons, hydroxyls, carbonate ions and alkali-metal the cathode anode to be managed, necessitating use ion-selective membranes regulate pH. Anion-exchange provide an alkaline environment, allowing low cell voltages suppression hydrogen evolution while maintaining high conversion efficiencies. However, local conditions presence alkali cations lead problematic formation even precipitation. Here we report pure-water-fed (alkali-cation-free) membrane–electrode–assembly system for ethylene by integrating anion-exchange membrane proton-exchange side, respectively, under forward bias. This effectively suppresses prevents salt A scaled-up electrolyser stack achieved over 1,000 h stability without electrolyte losses with 50% Faradaic efficiency towards total current 10 A.

Language: Английский

Citations

86
Single‐Product Faradaic Efficiency for Electrocatalytic of CO2 to CO at Current Density Larger than 1.2 A cm−2 in Neutral Aqueous Solution by a Single‐Atom Nanozyme DOI Open Access
Jia‐Run Huang,

Xiaofeng Qiu,

Zhen‐Hua Zhao

et al.

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 61(44)

Published: Sept. 7, 2022

Electroreduction of CO2 to CO is a promising approach for the cycling use , while it still suffers from impractical current density and durability. Here we report single-atom nanozyme (Ni-N5 -C) that achieves industrial-scale performance -to-CO conversion with Faradaic efficiency (FE) exceeded 97 % over -0.8--2.4 V vs. RHE. The at -2.4 RHE reached maximum 1.23 A cm-2 (turnover frequency 69.7 s-1 ) an FE 99.6 %. No obvious degradation was observed 100 hours continuous operation. Compared planar Ni-N4 site, square-pyramidal Ni-N5 site has increase decrease in dz2${{{\rm d}}_{{z}^{2}}}$ dxz/yz orbital energy levels, respectively, as revealed by functional theory calculations. Thus, catalytic more superior activate molecule reduce barriers well promote desorption, thus boosting kinetic activation process activity.

Language: Английский

Citations

84
Molecular Catalyst with Near 100% Selectivity for CO2 Reduction in Acidic Electrolytes DOI Open Access

Zhan Jiang,

Zisheng Zhang, Huan Li

et al.

Advanced Energy Materials, Journal Year: 2022, Volume and Issue: 13(6)

Published: Dec. 23, 2022

Abstract The electrocatalytic carbon dioxide reduction reaction (CO 2 RR) in an acidic medium is conducive to the efficient utilization of CO by preventing formation carbonate/bicarbonate. However, media are more favorable for hydrogen evolution (HER), resulting unsatisfactory RR selectivities. It demonstrated that molecularly dispersed electrocatalyst β‐tetra methoxy‐substituted nickel phthalocyanine on nanotubes (NiPc‐OMe MDE) can efficiently catalyze (pH 0.47) with Faradaic efficiencies >98% over a wide range current densities from −50 −400 mA cm −2 . found superior selectivity performance be attributed presence potassium ions, high preference HER active site, and few side sites. study illuminates potential molecular electrocatalysts selective rapid acid media.

Language: Английский

Citations

79
Continuous ammonia electrosynthesis using physically interlocked bipolar membrane at 1000 mA cm−2 DOI Creative Commons
Ziang Xu, Lei Wan,

Yiwen Liao

et al.

Nature Communications, Journal Year: 2023, Volume and Issue: 14(1)

Published: March 23, 2023

Abstract Electrosynthesis of ammonia from nitrate reduction receives extensive attention recently for its relatively mild conditions and clean energy requirements, while most existed electrochemical strategies can only deliver a low yield rate short duration the lack stable ion exchange membranes at high current density. Here, bipolar membrane process is proposed to achieve ionic balance, increasing water dissociation sites delivered by constructing three-dimensional physically interlocked interface membrane. This design simultaneously boosts transfer interfacial stability compared traditional ones, successfully reducing transmembrane voltage 1.13 V up density 1000 mA cm −2 . By combining Co nanoarray cathode designed large concentration utilizations, continuous reactor NH 3 electrosynthesis realized electrolysis over 100 h, Faradaic efficiency 86.2% maximum 68.4 mg h −1 with merely 2000 ppm NO - alkaline electrolyte. These results show promising potential artificial nitrogen cycling in near future.

Language: Английский

Citations

61
Reaction Environment Regulation for Electrocatalytic CO2 Reduction in Acids DOI
Min Zeng,

Wensheng Fang,

Yiren Cen

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(26)

Published: April 19, 2024

The electrocatalytic CO

Language: Английский

Citations

49
Understanding the complexity in bridging thermal and electrocatalytic methanation of CO2 DOI
Hui Kang, Jun Ma, Siglinda Perathoner

et al.

Chemical Society Reviews, Journal Year: 2023, Volume and Issue: 52(11), P. 3627 - 3662

Published: Jan. 1, 2023

The selective methanation of CO2 is an important research area to meet the net-zero emission targets. Furthermore, it crucial develop solutions achieve carbon neutrality, hydrogen utilization, circularity, and chemical-energy storage. This conversion can be realized via thermocatalytic multistep power-to-X route or by direct electro- (or photoelectro)-catalytic technologies. Herein, we discuss need accelerate Improving these technologies requires a better understanding catalytic chemistry complexity aspects consider in bridging electrocatalytic methanation. In this tutorial review, initially analyze fundamental question competitive adsorption key reactants regulation strategies promote overall reaction. Then, approach used guide reader differences between thermocatalysis electrocatalysis. Finally, necessary include modelling designing next-generation electrocatalysts for analyzed.

Language: Английский

Citations

46
Challenges and opportunities of atomic-scales reactive sites in thriving electrochemical CO2 reduction reaction DOI
Pengliang Sun, Sailin Liu, Xiong Zheng

et al.

Nano Today, Journal Year: 2024, Volume and Issue: 55, P. 102152 - 102152

Published: Jan. 13, 2024

Language: Английский

Citations

25
Addressing the Carbonate Issue: Electrocatalysts for Acidic CO2 Reduction Reaction DOI Creative Commons
Weixing Wu, Liangpang Xu, Qian Lü

et al.

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

Published: May 9, 2024

Abstract Electrochemical CO 2 reduction reaction (CO RR) powered by renewable energy provides a promising route to conversion and utilization. However, the widely used neutral/alkaline electrolyte consumes large amount of produce (bi)carbonate byproducts, leading significant challenges at device level, thereby impeding further deployment this reaction. Conducting RR in acidic electrolytes offers solution address “carbonate issue”; however, it presents inherent difficulties due competitive hydrogen evolution reaction, necessitating concerted efforts toward advanced catalyst electrode designs achieve high selectivity activity. This review encompasses recent developments RR, from mechanism elucidation design engineering. begins discussing mechanistic understanding pathway, laying foundation for RR. Subsequently, an in‐depth analysis advancements catalysts is provided, highlighting heterogeneous catalysts, surface immobilized molecular enhancement. Furthermore, progress made device‐level applications summarized, aiming develop high‐performance systems. Finally, existing future directions are outlined, emphasizing need improved selectivity, activity, stability, scalability.

Language: Английский

Citations

23