Technologies and perspectives for achieving carbon neutrality

The Innovation, Journal Year: 2021, Volume and Issue: 2(4), P. 100180 - 100180

Published: Oct. 30, 2021

Language: Английский

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Efficient Ammonia Electrosynthesis from Nitrate on Strained Ruthenium Nanoclusters

Journal of the American Chemical Society, Journal Year: 2020, Volume and Issue: 142(15), P. 7036 - 7046

Published: March 30, 2020

The limitations of the Haber-Bosch reaction, particularly high-temperature operation, have ignited new interests in low-temperature ammonia-synthesis scenarios. Ambient N2 electroreduction is a compelling alternative but impeded by low ammonia production rate (mostly <10 mmol gcat-1 h-1), small partial current density (<1 mA cm-2), and high-selectivity hydrogen-evolving side reaction. Herein, we report that room-temperature nitrate catalyzed strained ruthenium nanoclusters generates at higher (5.56 mol h-1) than process. primary contributor to such performance hydrogen radicals, which are generated suppressing hydrogen-hydrogen dimerization during water splitting enabled tensile lattice strains. radicals expedite nitrate-to-ammonia conversion hydrogenating intermediates rate-limiting steps lower kinetic barriers. nanostructures can maintain nearly 100% ammonia-evolving selectivity >120 cm-2 densities for 100 h due robust subsurface Ru-O coordination. These findings highlight potential real-world, synthesis.

Language: Английский

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Tailoring Acidic Oxygen Reduction Selectivity on Single-Atom Catalysts via Modification of First and Second Coordination Spheres

Journal of the American Chemical Society, Journal Year: 2021, Volume and Issue: 143(20), P. 7819 - 7827

Published: May 13, 2021

Product selectivity in multielectron electrocatalytic reactions is crucial to energy conversion efficiency and chemical production. However, a present practical drawback the limited understanding of actual catalytic active sites. Here, using as prototype single-atom catalysts (SACs) acidic oxygen reduction reaction (ORR), we report structure–property relationship show for first time that molecular-level local structure, including second coordination spheres (CSs), rather than individual atoms, synergistically determines response. ORR on Co-SACs can be tailored from four-electron two-electron pathway by modifying (N or/and O coordination) (C–O–C groups) CSs. Using combined theoretical predictions experiments, X-ray absorption fine structure analyses situ infrared spectroscopy, confirm unique change originates structure-dependent shift sites center Co atom O-adjacent C atom. We this optimizes electronic *OOH adsorption behavior give "best" activity >95% H2O2 electrosynthesis.

Language: Английский

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Cooperative CO2-to-ethanol conversion via enriched intermediates at molecule–metal catalyst interfaces

Nature Catalysis, Journal Year: 2019, Volume and Issue: 3(1), P. 75 - 82

Published: Dec. 16, 2019

Language: Английский

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Z‐Scheme Photocatalytic Systems for Carbon Dioxide Reduction: Where Are We Now?

Angewandte Chemie International Edition, Journal Year: 2020, Volume and Issue: 59(51), P. 22894 - 22915

Published: Feb. 3, 2020

Transforming CO2 into fuels by utilizing sunlight is promising to synchronously overcome global warming and energy-supply issues. It crucial design efficient photocatalysts with intriguing features such as robust light-harvesting ability, strong redox potential, high charge-separation, excellent durability. Hitherto, a single-component photocatalyst incapable simultaneously meet all these criteria. Inspired natural photosynthesis, constructing artificial Z-scheme provides facile way conquer bottlenecks. In this review, we firstly introduce the fundamentals of photocatalytic reduction systems. Thereafter discuss state-of-the-art reduction, whereby special attention placed on predominant factors that affect photoactivity. Additionally, further modifications are important for photocatalysis reviewed.

Language: Английский

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Electrocatalytic Refinery for Sustainable Production of Fuels and Chemicals

Angewandte Chemie International Edition, Journal Year: 2021, Volume and Issue: 60(36), P. 19572 - 19590

Published: Feb. 19, 2021

Abstract Compared to modern fossil‐fuel‐based refineries, the emerging electrocatalytic refinery (e‐refinery) is a more sustainable and environmentally benign strategy convert renewable feedstocks energy sources into transportable fuels value‐added chemicals. A crucial step in conducting e‐refinery processes development of appropriate reactions optimal electrocatalysts for efficient cleavage formation chemical bonds. However, compared well‐studied primary (e.g., O 2 reduction, water splitting), mechanistic aspects materials design complex are yet be settled. To address this challenge, herein, we first present fundamentals heterogeneous electrocatalysis some reactions, then implement these establish framework by coupling situ generated intermediates (integrated reactions) or products (tandem reactions). We also set principles strategies efficiently manipulate reaction pathways.

Language: Английский

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Operando studies reveal active Cu nanograins for CO2 electroreduction

Nature, Journal Year: 2023, Volume and Issue: 614(7947), P. 262 - 269

Published: Feb. 8, 2023

Language: Английский

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Heterogeneous Single‐Atom Catalysts for Electrochemical CO₂ Reduction Reaction

Advanced Materials, Journal Year: 2020, Volume and Issue: 32(34)

Published: July 9, 2020

The electrochemical CO2 reduction reaction (CO2 RR) is of great importance to tackle the rising concentration in atmosphere. RR can be driven by renewable energy sources, producing precious chemicals and fuels, with implementation this process largely relying on development low-cost efficient electrocatalysts. Recently, a range heterogeneous potentially single-atom catalysts (SACs) containing non-precious metals coordinated earth-abundant elements have emerged as promising candidates for RR. Unfortunately, real catalytically active centers key factors that govern catalytic performance these SACs remain ambiguous. Here, ambiguity addressed developing fundamental understanding RR-to-CO SACs, CO accounts major product from SACs. mechanism, rate-determining steps, control activity selectivity are analyzed both experimental theoretical studies. Then, synthesis, characterization, discussed. Finally, challenges future pathways highlighted hope guiding design promote understand

Language: Английский

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Enhancing carbon dioxide gas-diffusion electrolysis by creating a hydrophobic catalyst microenvironment

Nature Communications, Journal Year: 2021, Volume and Issue: 12(1)

Published: Jan. 8, 2021

Electroreduction of carbon dioxide (CO

Language: Английский

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Gas diffusion electrodes and membranes for CO2 reduction electrolysers

Nature Reviews Materials, Journal Year: 2021, Volume and Issue: 7(1), P. 55 - 64

Published: Sept. 17, 2021

Language: Английский

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