Stabilizing the oxidation state of catalysts for effective electrochemical carbon dioxide conversion

Chemical Society Reviews, Год журнала: 2024, Номер 53(12), С. 6295 - 6321

Опубликована: Янв. 1, 2024

Developing sophisticated strategies to stabilize oxidative metal catalysts based on the correlation between dynamic oxidation state and product profile is favorable for efficient electrochemical CO 2 conversion.

Язык: Английский

---

Continuously Producing Highly Concentrated and Pure Acetic Acid Aqueous Solution via Direct Electroreduction of CO₂

Journal of the American Chemical Society, Год журнала: 2024, Номер 146(1), С. 1144 - 1152

Опубликована: Янв. 2, 2024

It is crucial to achieve continuous production of highly concentrated and pure C2 chemicals through the electrochemical CO2 reduction reaction (eCO2RR) for artificial carbon cycling, yet it has remained unattainable until now. Despite one-pot tandem catalysis (dividing eCO2RR into two catalytical reactions CO C2) offering potential significantly enhancing efficiency, its mechanism remains unclear performance unsatisfactory. Herein, we selected different CO2-to-CO catalysts CO-to-acetate construct several catalytic systems acetic acid. Among them, a system comprising covalent organic framework (PcNi-DMTP) metal–organic (MAF-2) as catalysts, respectively, exhibited faradaic efficiency 51.2% with current density 410 mA cm–2 an ultrahigh acetate yield rate 2.72 mmol m–2 s–1 under neutral conditions. After electrolysis 200 h, 1 working electrode can continuously produce 20 mM acid aqueous solution relative purity 95+%. Comprehensive studies revealed that influenced not only by supply–demand relationship electron competition between processes in but also CO-to-C2 catalyst diluted

Язык: Английский

---

Current Status and Perspectives of Dual-Atom Catalysts Towards Sustainable Energy Utilization

Nano-Micro Letters, Год журнала: 2024, Номер 16(1)

Опубликована: Фев. 29, 2024

Abstract The exploration of sustainable energy utilization requires the implementation advanced electrochemical devices for efficient conversion and storage, which are enabled by usage cost-effective, high-performance electrocatalysts. Currently, heterogeneous atomically dispersed catalysts considered as potential candidates a wide range applications. Compared to conventional catalysts, metal atoms in carbon-based have more unsaturated coordination sites, quantum size effect, strong metal–support interactions, resulting exceptional catalytic activity. Of these, dual-atomic (DACs) attracted extensive attention due additional synergistic effect between two adjacent atoms. DACs advantages full active site exposure, high selectivity, theoretical 100% atom utilization, ability break scaling relationship adsorption free on sites. In this review, we summarize recent research advancement DACs, includes (1) comprehensive understanding synergy atomic pairs; (2) synthesis DACs; (3) characterization methods, especially aberration-corrected scanning transmission electron microscopy synchrotron spectroscopy; (4) energy-related last part focuses great catalysis small molecules, such oxygen reduction reaction, CO 2 hydrogen evolution N reaction. future challenges opportunities also raised prospective section.

Язык: Английский

---

Bimetallic Single-Atom Catalysts for Water Splitting

Nano-Micro Letters, Год журнала: 2024, Номер 17(1)

Опубликована: Сен. 25, 2024

Abstract Green hydrogen from water splitting has emerged as a critical energy vector with the potential to spearhead global transition fossil fuel-independent society. The field of catalysis been revolutionized by single-atom catalysts (SACs), which exhibit unique and intricate interactions between atomically dispersed metal atoms their supports. Recently, bimetallic SACs (bimSACs) have garnered significant attention for leveraging synergistic functions two ions coordinated on appropriately designed BimSACs offer an avenue rich metal–metal metal–support cooperativity, potentially addressing current limitations in effectively furnishing transformations involve synchronous proton–electron exchanges, substrate activation reversible redox cycles, simultaneous multi-electron transfer, regulation spin states, tuning electronic properties, cyclic states low energies. This review aims encapsulate growing advancements bimSACs, emphasis pivotal role generation via splitting. We subsequently delve into advanced experimental methodologies elaborate characterization SACs, elucidate discuss local coordination environment. Overall, we present comprehensive discussion deployment bimSACs both evolution reaction oxygen reaction, half-reactions electrolysis process.

Язык: Английский

---

Metal-organic framework-derived diatomic catalysts for environmental remediation: Synthesis, applications and improvement strategies

Coordination Chemistry Reviews, Год журнала: 2024, Номер 526, С. 216357 - 216357

Опубликована: Ноя. 29, 2024

Язык: Английский

---

Symmetry Evolution Induced 2D Pt Single Atom Catalyst with High Density for Alkaline Hydrogen Oxidation

Advanced Materials, Год журнала: 2024, Номер 36(31)

Опубликована: Апрель 18, 2024

The performance of single-atom catalysts is greatly influenced by the chemical environment surrounding central atom. Here, a salt-assisted method employed to transform tetrahedral coordination structure zeolitic imidazolate frameworks - 8 (ZIF-8) into planar square without altering ligands. During subsequent carbonization process, concurrent with evaporation zinc atoms, nitrogen and carbon carriers (NC carriers) undergoes transition from five-membered rings six-membered preserve 2D structure. This results in generation additional defect sites on 2D-NC substrates. Hence, Pt symmetries can be precisely prepared via electrodeposition (denoted as 2D-Pt SAC). loading SAC 0.49 ± 0.03 µg cm

Язык: Английский

---

Recent advances and challenges of double-atom catalysts in diverse environmental applications: A state-of-the-art review

Coordination Chemistry Reviews, Год журнала: 2025, Номер 532, С. 216545 - 216545

Опубликована: Фев. 19, 2025

Язык: Английский

---

Sulfur-doping tunes p-d orbital coupling over asymmetric Zn-Sn dual-atom for boosting CO2 electroreduction to formate

Nature Communications, Год журнала: 2025, Номер 16(1)

Опубликована: Март 5, 2025

The interaction of p-d orbitals at bimetallic sites plays a crucial role in determining the catalytic reactivity, which facilitates modulation charges and enhances efficiency CO2 electroreduction process. Here, we show ligand co-etching approach to create asymmetric Zn-Sn dual-atom (DASs) within metal-organic framework (MOF)-derived yolk-shell carbon frameworks (named Zn1Sn1/SNC). DASs comprise one Sn center (p-block) partially doped with sulfur Zn (d-block) N coordination, facilitating coupling between dimer. N-Zn-Sn-S/N arrangement displays an distribution atoms, leading stable adsorption configuration HCOO* intermediates. In H-type cell, Zn1Sn1/SNC exhibits impressive formate Faraday 94.6% -0.84 V. flow electronic architecture high accessibility, current density -315.2 mA cm-2 -0.90 Theoretical calculations ideal affinity lower reduction barrier, thus improve overall reduction.

Язык: Английский

---

Targeting Synthesis of Diatomic Catalysts by Selective Etching and Sequential Adsorption of Metal Atom

Journal of the American Chemical Society, Год журнала: 2025, Номер unknown

Опубликована: Янв. 8, 2025

Diatomic catalysts featuring a tunable structure and synergetic effects hold great promise for various reactions. However, their precise construction with specific configurations diverse metal combinations is still challenging. Here, selective etching ion adsorption strategy proposed to accurately assign second atom (M2) geminal the single site (M1–Nx) constructing diatomic sites (e.g., Fe–Pd, Fe–Pt, Fe–Ru, Fe–Zn, Co–Fe, Co–Ni, Co–Cu). In this strategy, hydrogen peroxide selectively etches positively charged carbon atoms near M1–Nx moiety (denoted as α-C) produces vacancy, which could trap M2 at subsequent step. These show optimized electronic enhanced oxygen reduction activity compared single-site counterparts, representative Fe–Pd–NC Co–Fe–NC stand most active reaction (half-wave potential of 0.92 0.91 V, respectively). The α-C in single-atom reported here represents new post-treatment targeting synthesis sites.

Язык: Английский

---

Advanced Catalyst Design and Reactor Configuration Upgrade in Electrochemical Carbon Dioxide Conversion

Advanced Materials, Год журнала: 2023, Номер 35(52)

Опубликована: Авг. 20, 2023

Abstract Electrochemical carbon dioxide reduction reaction (CO 2 RR) driven by renewable energy shows great promise in mitigating and potentially reversing the devastating effects of anthropogenic climate change environmental degradation. The simultaneous synthesis energy‐dense chemicals can meet global demand while decoupling emissions from economic growth. However, development CO RR technology faces challenges catalyst discovery device optimization that hinder their industrial implementation. In this contribution, a comprehensive overview current state research is provided, starting with background motivation for technology, followed fundamentals evaluated metrics. Then underlying design principles electrocatalysts are discussed, emphasizing structure–performance correlations advanced electrochemical assembly cells increase selectivity throughput. Finally, review looks to future identifies opportunities innovation mechanism discovery, material screening strategies, assemblies move toward carbon‐neutral society.

Язык: Английский

---