Transient pulsed discharge preparation of graphene aerogel supports asymmetric Cu cluster catalysts promote CO2 electroreduction

Nature Communications, Journal Year: 2025, Volume and Issue: 16(1)

Published: Jan. 31, 2025

Designing asymmetrical structures is an effective strategy to optimize metallic catalysts for electrochemical carbon dioxide reduction reactions. Herein, we demonstrate a transient pulsed discharge method instantaneously constructing graphene-aerogel supports asymmetric copper nanocluster catalysts. This process induces the convergence of atoms decomposed by chloride onto graphene originating from intense current pulse and high temperature. The exhibit atomic electronic due lattice distortion oxygen doping clusters. In reaction, selectivity activity ethanol production are enhanced structure abundance active sites on catalysts, achieving Faradaic efficiency 75.3% 90.5% multicarbon products at −1.1 V vs. reversible hydrogen electrode. Moreover, strong interactions between nanoclusters support confer notable long-term stability. We elucidate key reaction intermediates mechanisms Cu4O-Cu/C2O1 moieties through in situ testing density functional theory calculations. study provides innovative approach balancing stability asymmetric-structure energy conversion. Asymmetric show promise CO2 catalytic reduction. Here, authors develop prepare graphene-aerogel-supported Cu that enhance conversion into products.

Language: Английский

---

Cu–Sb Atomic Pair Site in Metal Halide Perovskite for CO₂ Reduction to Methanol

Inorganic Chemistry, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 24, 2025

Electrochemical conversion of CO2 into methanol has received extensive attention in recent years since is an efficient energy carrier and industrial feedstock. However, the selectivity to remains unsatisfied. In this work, Sb-doped Cs3Cu2I5 first rationally developed for electrochemical reduction, achieving remarkable high methanol. UV–vis absorption, X-ray photoelectron spectroscopy (XPS), density functional theory (DFT) calculations show that Sb dopants narrow band gap enhance metal–ligand hybridization due introduction 5p orbitals, which accordingly charge transfer. addition, Cu–Sb pair Sb@Cs3Cu2I5 perovskite synergistically catalyzes conversion. The Cu sites serve absorption activation, while stabilize intermediate *OCH2 through Sb–O bond superior oxygen affinity. plasma-treated sample with electron-deficient exhibits best as 88.38%. This work provides new insight highly metal halide perovskite-based catalysts

Language: Английский

---

Microenvironment Matters: Copper–Carbon Composites Enable a Highly Efficient Carbon Dioxide Reduction Reaction to C₂ Products

ACS Applied Materials & Interfaces, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 4, 2025

Copper is the catalyst widely used to produce multicarbon products for carbon dioxide reduction reaction (CO2RR). The surrounding microenvironment of copper plays a crucial role in determining its catalytic activity and selectivity. In this study, we compare three electrocatalysts with different microenvironments: pure metallic copper, metal–organic framework (MOF), MOF-derived copper–carbon composite. Operando X-ray absorption spectroscopy, transmission electron microscopy, Raman spectroscopy reveal that composite remains state, encapsulated by matrix. achieves Faradaic efficiency 75.6% C2 products, including ethylene ethanol, at current density 500 mA cm–2, 377.9 cm–2. This performance suppresses which reaches an optimal 64.5% 300 193.5 also significantly overperforms copper-MOF catalyst, shows 52.0% 400 208.0 These findings highlight importance near active sites CO2RR efficiency. We hope our results provide valuable insights advancing design reduction, contributing reduced emissions improved environmental sustainability.

Language: Английский

---

Confining asymmetric water hydrogen-bond network to boost photoreduction of CO2 to formaldehyde

Chemical Engineering Journal, Journal Year: 2025, Volume and Issue: unknown, P. 161232 - 161232

Published: March 1, 2025

Language: Английский

---

Stretchable asymmetric dual-atom Cu(I) electrocatalyst for enhanced CO2 reduction to C2+ products

Chem Catalysis, Journal Year: 2025, Volume and Issue: unknown, P. 101327 - 101327

Published: March 1, 2025

Language: Английский

---

Highly Selective Electroreduction of CO₂ to CH₄ on Cu–Pd Alloy Catalyst: the Role of Palladium‐Adsorbed Hydrogen Species and Blocking Effect

Advanced Science, Journal Year: 2025, Volume and Issue: unknown

Published: March 26, 2025

Electroreduction of CO2 to chemical fuels offers a promising strategy for controlling the global carbon balance and addressing need storage intermittent renewable energy. In this work, it is demonstrated that tuning adjacent active sites enables selection different reaction pathways generating C1 or C2 products during electroreduction CO2. Cu Cu-Pd alloy catalysts with atomic ratios are synthesized investigated elucidate their selectivities electroreduction. catalyst favors formation since neighboring beneficial coupling adjacently adsorbed *CO *CHO intermediates. alloyed Pd introduces blocking effect increases intermolecular distance between Therefore selectivity C2H4 pathway decreas while CH4 enhanced. Moreover, existence *H species on atoms also played significant role in boosting by facilitating hydrogenation This work reveals key formation, which helpful design copper-based desired products.

Language: Английский

---

Artificial Photothermal Synthesis of Hydrocarbons from CO₂ and H₂O

Advanced Energy Materials, Journal Year: 2025, Volume and Issue: unknown

Published: April 22, 2025

Abstract The excessive release of CO 2 from fossil fuel combustion has disrupted the carbon cycle, leading to elevated greenhouse gas levels. Converting into value‐added chemicals like CH 4 and C H not only offers a sustainable alternative fuels but also helps mitigate emissions. However, producing high‐energy hydrocarbons involves complex electron proton coupling, presenting significant kinetic challenges. Photothermal catalysis, which harnesses solar energy in light heat, emerges as promising method for efficient conversion hydrocarbons. This process reduces thermodynamic barriers protonation by enabling rapid transfer through thermal assistance. development photothermal catalysts capable absorbing light, generating electron–hole pairs, facilitating redox reactions is crucial enhancing efficiency selectivity. review highlights importance catalyst design, reaction conditions, reactor configuration, addresses lack comprehensive reviews on synergistic approach catalysis. By focusing precise design photogenerated heat mechanisms, this aims advance field, emphasizing its potential promote carbon‐neutral future.

Language: Английский

---

Hierarchical Assembly of High-Nuclearity Copper(I) Alkynide Nanoclusters: Highly Effective CO₂ Electroreduction Catalyst toward Hydrocarbons

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: unknown

Published: Oct. 4, 2024

The pursuit of precision in the engineering metal nanoparticle assemblies has long fascinated scientists, but achieving atomic-level accuracy continues to pose a significant challenge. This research sheds light on hierarchical assembly processes two high-nuclearity Cu(I) nanoclusters (NCs). By employing multiligand cooperative stabilization strategy, we have isolated series thiacalix[4]arene (TC4A)/alkynyl coprotected NCs (

Language: Английский

---

Highly Efficient Stable Pyroglutamic Acid-Modified Cu2O/Cu Catalysts with Reconstruction-resistant Interfaces for CO2-to-C2 Conversion at High Current Density

Applied Catalysis B Environment and Energy, Journal Year: 2024, Volume and Issue: unknown, P. 124977 - 124977

Published: Dec. 1, 2024

Language: Английский

---