High‐rate CO2‐to‐CH4 Electrosynthesis by Undercoordinated Cu Sites in Alkaline‐Earth‐Metal Perovskites with Strong Basicity DOI
Zikai Xu, Peng Chen, Gan Luo

et al.

Advanced Energy Materials, Journal Year: 2023, Volume and Issue: 13(19)

Published: April 9, 2023

Abstract The electrochemical CO 2 reduction to CH 4 has been extensively demonstrated, but still suffers from relatively poor activity and requires high overpotentials especially at large electrolysis rates. Perovskite oxides (A x B y O) are one type of promising electrocatalyst for the due their tunable electronic structures. In this work, a Ca CuO 3 perovskite oxide catalyst is developed with alkaline‐earth A‐sites, featuring an inherently strong basic strengthand outstanding capability adsorption, as well undercoordinated Cu sites generated through partial surface 2+ cation leaching. exhibitsa current density 517 ± 23 mA cm −2 producing low applied potential −0.30 V versus reversible hydrogen electrode, which further reached peak value 1452 156 . Density functional calculations show that allowed promote hydrogenation * subsequent CHO intermediates, thus leading activity. This work suggests attractive design strategy tuning A‐sites in realize high‐rate ‐to‐CH electrosynthesis overpotentials.

Language: Английский

Turning Carbon Dioxide into Sustainable Food and Chemicals: How Electrosynthesized Acetate Is Paving the Way for Fermentation Innovation DOI
Bradie S. Crandall, Sean Overa, Haeun Shin

et al.

Accounts of Chemical Research, Journal Year: 2023, Volume and Issue: 56(12), P. 1505 - 1516

Published: May 19, 2023

The agricultural and chemical industries are major contributors to climate change. To address this issue, hybrid electrocatalytic-biocatalytic systems have emerged as a promising solution for reducing the environmental impact of these key sectors while providing economic onboarding carbon capture technology. Recent advancements in production acetate via CO2/CO electrolysis well advances precision fermentation technology prompted electrochemical be explored an alternative source synthetic biology. Tandem CO2 coupled with improved reactor design has accelerated commercial viability electrosynthesized recent years. Simultaneously, innovations metabolic engineering helped leverage pathways that facilitate upgrading higher carbons sustainable food fermentation. Current received much criticism reliance upon crop-derived sugars starches feedstock which compete human chain. A shift toward feedstocks could help preserve arable land rapidly growing population.Technoeconomic analysis shows using instead glucose reduces costs chemicals by 16% offers market price stability. Moreover, given rapid decline utility-scale renewable electricity prices, electro-synthesized may become more affordable than conventional methods at scale. This work provides outlook on strategies further advance scale-up production. Additional perspective is offered ensure successful integration technologies. In electrocatalytic step, it critical relatively high purity can produced low-concentration electrolyte minimal treatment stream needed prior biocatalytic microbes increased tolerances elevated concentrations engineered promote uptake accelerate product formation. Additionally, tighter regulation metabolism strain essential improving cellular efficiency. implementation would allow coupling offer approach sustainably produce food. Reducing necessary avoid catastrophe habitability planet future generations.

Language: Английский

Citations

25
Electrosynthesis of ethylene glycol from C1 feedstocks in a flow electrolyzer DOI Creative Commons
Rong Xia, Ruoyu Wang, Bjorn Hasa

et al.

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

Published: July 29, 2023

Abstract Ethylene glycol is a widely utilized commodity chemical, the production of which accounts for over 46 million tons CO 2 emission annually. Here we report paired electrocatalytic approach ethylene from methanol. Carbon catalysts are effective in reducing formaldehyde into with 92% Faradaic efficiency, whereas Pt at anode enable through methanol partial oxidation 75% efficiency. With membrane-electrode assembly configuration, show feasibility electrosynthesis single electrolyzer. The electrolyzer operates full cell voltage 3.2 V current density 100 mA cm −2 , 60% reduction energy consumption. Further investigations, using operando flow mass spectroscopy, isotopic labeling, and functional theory (DFT) calculations, indicate that desorption *CH OH intermediate crucial step determining selectively towards

Language: Английский

Citations

23
Efficient ethylene electrosynthesis through C–O cleavage promoted by water dissociation DOI
Yongxiang Liang, Feng Li, Rui Kai Miao

et al.

Nature Synthesis, Journal Year: 2024, Volume and Issue: 3(9), P. 1104 - 1112

Published: June 20, 2024

Language: Английский

Citations

16
Efficient C–N coupling for urea electrosynthesis on defective Co3O4 with dual-functional sites DOI Creative Commons
Pengsong Li, Qinggong Zhu, Jiyuan Liu

et al.

Chemical Science, Journal Year: 2024, Volume and Issue: 15(9), P. 3233 - 3239

Published: Jan. 1, 2024

Defective Co 3 O 4 catalysts featuring dual-functional sites were synthesized using a facile thermal annealing strategy to enhance the adsorption of reactants/intermediates and facilitate effective C–N coupling for urea production from CO 2 nitrite.

Language: Английский

Citations

14
Models for Decarbonization in the Chemical Industry DOI
Yuan Yao, Kai Lan, T. E. Graedel

et al.

Annual Review of Chemical and Biomolecular Engineering, Journal Year: 2024, Volume and Issue: 15(1), P. 139 - 161

Published: Jan. 25, 2024

Various technologies and strategies have been proposed to decarbonize the chemical industry. Assessing decarbonization, environmental, economic implications of these is critical identifying pathways a more sustainable industrial future. This study reviews recent advancements integration systems analysis models, including process analysis, material flow life cycle assessment, techno-economic machine learning. These models are categorized based on analytical methods application scales (i.e., micro-, meso-, macroscale) for promising decarbonization (e.g., carbon capture, storage, utilization, biomass feedstock, electrification) circular economy strategies. Incorporating forward-looking, data-driven approaches into existing allows optimizing complex assessing future impacts. Although advances in ecology–, economic-, planetary boundary–based modeling support holistic systems-level efforts needed consider impacts ecosystems. Effective applications advanced, integrated require cross-disciplinary collaborations across engineering, ecology, economics.

Language: Английский

Citations

13
Fabrication of vanadium telluride anchored on carbon nanotubes nanocomposite for overall water splitting DOI
Nigarish Bano, Sumaira Manzoor,

Abdus Sami

et al.

Journal of the American Ceramic Society, Journal Year: 2024, Volume and Issue: 107(6), P. 4027 - 4041

Published: Jan. 29, 2024

Abstract Electrocatalytic water splitting is an essential hydrogen production method for resolving present energy shortage and progress toward more efficient technologies. For this purpose, a versatile cheap electrocatalysts are the main challenge along way. In report, we synthesized vanadium telluride carbon nanotube (VTe–CNT)‐based nanocomposite via facile hydrothermal route. The VTe–CNTs characterized by X‐ray diffraction analysis, scanning electron microscopy, energy‐dispersive spectroscopy, Fourier transform infrared Brunauer–Emmett–Teller. These characterizations depict nanosphere structures, morphology, high surface area that maintains porosity, which inclusive water‐splitting phenomena in 1.0 M solution of KOH. Additionally, electrochemical performance has shown best O 2 evolution reactions activity with onset potential 1.42 V versus reversible electrode required 10 mA/cm current density at 278 mV overpotential, excellent among other electrocatalysts, VTe (342 mV@10 −2 ) CNTs (365 mV@10mA/cm ). Moreover, VTe–CNT exhibits remarkable stability almost 20 h. It also requires low 0.05 small Tafel slope 47 mV/dec H reactions. Hence, research might facilitate easy transportation electrons open up new era, serving as replacement noble metal–derived materials.

Language: Английский

Citations

12
Catalysis of C-N Coupling on High-Entropy Alloys DOI Creative Commons
Mads K. Plenge, Jack K. Pedersen, Alexander Bagger

et al.

Journal of Catalysis, Journal Year: 2024, Volume and Issue: 430, P. 115322 - 115322

Published: Jan. 26, 2024

Catalyzing carbon–nitrogen (C-N) coupling using small abundant nitrogenous molecules is of growing interest to lessen the environmental impact industrial process. High-entropy alloys hold potential have surface sites optimized for each intermediates and by varying alloy composition catalyst it provides tunability adsorption energy distribution. We model C-N energies CO NO assume that *CO couples with an *NO-reduced intermediate. As more mechanistic inside needed, we limit coverage pairs *NO, providing a necessary but not sufficient condition catalytic activity. Two limiting cases simulating process are presented: one considering thermodynamic equilibrium out-of-equilibrium conditions. A Monte Carlo method connecting two limits suggested which reproduce trends observed in experiments. By partial pressure shape pair function space as well its optima altered. Our finds ternary AuCuPd optimum at equal CO/NO pressures copper be low pressures.

Language: Английский

Citations

9
Electrochemical regeneration of high-purity CO2 from (bi)carbonates in a porous solid electrolyte reactor for efficient carbon capture DOI
Xiao Zhang, Zhiwei Fang, Peng Zhu

et al.

Nature Energy, Journal Year: 2024, Volume and Issue: unknown

Published: Oct. 11, 2024

Language: Английский

Citations

9
The costs of future energy technologies: A comprehensive review of power-to-X processes DOI Creative Commons
G. Müller, Felix Kullmann, Jochen Linßen

et al.

Journal of CO2 Utilization, Journal Year: 2025, Volume and Issue: 92, P. 103019 - 103019

Published: Jan. 11, 2025

Language: Английский

Citations

1
Predicting electrocatalytic urea synthesis using a two-dimensional descriptor DOI Creative Commons
Amy Wuttke, Alexander Bagger

Communications Chemistry, Journal Year: 2025, Volume and Issue: 8(1)

Published: Feb. 3, 2025

Electrochemical synthesis routes powered by renewable electricity can provide sustainable chemical commodities replacing conventional fossil-based processes. Increasing research focuses on value-added chemicals like the indispensable fertilizer urea, which also constitutes a study case for electrochemical CN-coupling. To guide identification of highly selective catalysts, we aim to new insight analysing existing experimental data selectivity transition metal catalysts towards electrochemically synthesized urea. Firstly, project high dimensional using principal component analysis (PCA) lower dimensions, and thereby confirm that urea is correlated with CO NH3. Furthermore, identified most suitable two-dimensional descriptors prediction out various adsorption energies calculated density functional theory (DFT). We suggest *H *O slabs predict in co-reduction CO2 nitrite ( NO2- ).

Language: Английский

Citations

1