Low-Cost, Facile, and Scalable Manufacturing of Single-Molecule-Integrated Catalytic Electrodes

ACS Nano, Journal Year: 2025, Volume and Issue: unknown

Published: March 12, 2025

To surmount the shortcomings of powder-based catalysts and small electrode sizes, development meter-scale integrated materials is essential for practical electrocatalytic applications, which requires fine control over effective surface grafting catalytic active sites on large-size electrodes as well addressing challenge balancing cost-effective large-scale manufacturing with highly stable operation. Herein, we report a low-cost, facile, scalable method directly constructing single-molecule-integrated using commercially available, flexible, size-tailored conductive carbon textiles (e.g., graphite felt) well-defined planar conjugated molecules metallophthalocyanines) via heterostacking steered cross-scale heterointerfacial assembly. This universal unlocks limitations traditional approaches that involve integrating catalysts, particles, binders Nafion), supported paper) through multiple processing steps typically result in centimeter-level electrodes. Meaningfully, our enables precise size, composition, microenvironment, structure to match various environments. As proof concept, an thiophene-gilded cobalt phthalocyanine demonstrates outstanding activity stability CO2 electroconversion alkaline, neutral, acidic media under industrially relevant current densities, even flowing paired-electrolysis system. study provides comprehensive scientific data engineering guidance systematic design scalable, binder-free electrodes, thereby promising drive sustainable energy-efficient electrolysis industrial scene.

Language: Английский

---

Identifying Highly Active and Selective Cobalt X‐Ides for Electrocatalytic Hydrogenation of Quinoline

Advanced Materials, Journal Year: 2024, Volume and Issue: 36(41)

Published: Sept. 2, 2024

Abstract Earth‐abundant Co X‐ides are emerging as promising catalysts for the electrocatalytic hydrogenation of quinoline (ECHQ), yet challenging due to limited fundamental understanding ECHQ mechanism on X‐ides. This work identifies catalytic performance differences in and provides significant insights into ECHQ. Among selected X‐ides, 3 O 4 presents best with a high conversion 98.2% 100% selectivity at ambient conditions. The sites present higher proportion 2‐coordinated hydrogen‐bonded water interface than other low negative potential, which enhances kinetics subsequent dissociation produce H*. An ideal 1,4/2,3‐H* addition pathway surface spontaneous desorption 1,2,3,4‐tetrahydroquinoline is demonstrated through operando tracing theoretical calculations. In comparison, 9 S 8 display lowest thermodynamic barrier H* formation step, suppresses hydrogenation; while Co(OH)F CoP undergo 1,2,3,4‐ 4,3/1,2‐H* respectively barriers thus quinoline. Moreover, wide substrate scope allows excellent derivatives N ‐heterocyclic substrates.

Language: Английский

---

Modified Cu active sites by alloying for efficient electrocatalytic reduction CO2 to CO

Journal of Energy Chemistry, Journal Year: 2024, Volume and Issue: 99, P. 450 - 457

Published: Aug. 12, 2024

Language: Английский

---

Solid Electrolytes for Low-Temperature Carbon Dioxide Valorization: A Review

Environmental Science & Technology, Journal Year: 2024, Volume and Issue: 58(25), P. 10881 - 10896

Published: June 11, 2024

One of the most promising approaches to address global challenge climate change is electrochemical carbon capture and utilization. Solid electrolytes can play a crucial role in establishing chemical-free pathway for CO2. Furthermore, they be applied electrocatalytic CO2 reduction reactions (CO2RR) increase utilization, produce high-purity liquid chemicals, advance hybrid electro-biosystems. This review article begins by covering fundamentals processes capture, emphasizing advantages utilizing solid electrolytes. Additionally, it highlights recent advancements use polymer electrolyte or layer CO2RR with multiple functions. The also explores avenues future research fully harness potential electrolytes, including integration performance assessment under realistic conditions. Finally, this discusses opportunities challenges, aiming contribute establishment green sustainable society through valorization.

Language: Английский

---

Species mass transfer governs the selectivity of gas diffusion electrodes toward H2O2 electrosynthesis

Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)

Published: Dec. 5, 2024

The meticulous design of advanced electrocatalysts and their integration into gas diffusion electrode (GDE) architectures is emerging as a prominent research paradigm in the H2O2 electrosynthesis community. However, it remains perplexing that assembled GDE frequently exhibit substantial discrepancies selectivity during bulk electrolysis. Here, we elucidate pivotal role mass transfer behavior key species (including reactants products) beyond intrinsic properties electrocatalyst dictating electrode-scale selectivity. This tendency becomes more pronounced high reaction rate (current density) regimes where transport limitations are intensified. By utilizing diffusion-related parameters (DRP) GDEs (i.e., wettability catalyst layer thickness) probe factors, employ both short- long-term electrolysis conjunction with in-situ electrochemical reflection-absorption imaging theoretical calculations to thoroughly investigate impact DRP DRP-controlled local microenvironments on O2 transfer. mechanistic origins diffusion-dependent conversion at scale unveiled accordingly. fundamental insights gained from this study underscore necessity architectural innovations for mainstream hydrophobic can synchronously optimize products, paving way next-generation gas-consuming electroreduction scenarios. Electrocatalysts electrodes electrosynthesis. authors report

Language: Английский

---

Strong effect-correlated electrochemical CO₂ reduction

Chemical Society Reviews, Journal Year: 2024, Volume and Issue: 53(18), P. 9344 - 9377

Published: Jan. 1, 2024

Electrochemical CO

Language: Английский

---

Reaction Environment Regulation for Electrocatalytic CO₂ Reduction in Acids

Angewandte Chemie, Journal Year: 2024, Volume and Issue: 136(26)

Published: April 19, 2024

Abstract The electrocatalytic CO 2 reduction reaction (CO RR) is a sustainable route for converting into value‐added fuels and feedstocks, advancing carbon‐neutral economy. electrolyte critically influences utilization, rate product selectivity. While typically conducted in neutral/alkaline aqueous electrolytes, the RR faces challenges due to (bi)carbonate formation its crossover anolyte, reducing efficiency stability. Acidic media offer promise by suppressing these processes, but low Faradaic efficiency, especially multicarbon (C 2+ ) products, poor electrocatalyst stability persist. effective regulation of environment at cathode essential favor over competitive hydrogen evolution (HER) improve long‐term This review examines progress acidic RR, focusing on strategies such as design, electrode modification engineering promote RR. Insights mechanisms via situ/operando techniques theoretical calculations are discussed, along with critical future directions technology, offering guidance developing practical systems community.

Language: Английский

---

Modulating Electronic Properties of Carbon for Selective Electrochemical Reduction of CO₂ to Methanol on Cu₃P@C

ACS Catalysis, Journal Year: 2024, Volume and Issue: 14(17), P. 12783 - 12791

Published: Aug. 9, 2024

Carbon layer-coated CuX (CuX@C, X = P, S, Se) with different electron densities on the carbon coating layers have been successfully prepared. Among them, Cu3P@C, which has a high-electron-density layer, delivers high faradaic efficiency for methanol of 61.2% at −0.36 V versus reversible hydrogen electrode (RHE), and record partial current density 130 mA cm–2 −0.76 RHE when it is assembled gas diffusion in flow cell setup using 1 M KOH electrolyte, outperforming most state-of-the-art electrocatalysts. In contrast, Cu2Se@C Cu1.8S@C, low-electron-density layers, predominately produce formate. situ Raman spectroscopy analysis computational functional theory calculations reveal influence Cu3P electronic properties binding sites underlying mechanisms production.

Language: Английский

---

Catalyst Design and Engineering for CO₂‐to‐Formic Acid Electrosynthesis for a Low‐Carbon Economy

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

Published: Oct. 12, 2024

Abstract Formic acid (FA) has emerged as a promising candidate for hydrogen energy storage due to its favorable properties such low toxicity, flammability, and high volumetric capacity under ambient conditions. Recent analyses have suggested that FA produced by electrochemical carbon dioxide (CO 2 ) reduction reaction (eCO RR) using low‐carbon electricity exhibits lower fugitive (H emissions global warming potential (GWP) during the H carrier production, transportation processes compared those of other alternatives like methanol, methylcyclohexane, ammonia. eCO RR can enable industrially relevant current densities without need pressures, temperatures, or auxiliary sources. However, widespread implementation is hindered requirement highly stable selective catalysts. Herein, aim explore evaluate catalyst engineering in designing nanostructured catalysts facilitate economically viable production FA.

Language: Английский

---

Electrochemical In Situ Characterization Techniques in the Field of Energy Conversion

Small Methods, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 9, 2025

Abstract With the proposal of “carbon peak and carbon neutrality” goals, utilization renewable energy sources such as solar energy, wind tidal has garnered increasing attention. Consequently, development corresponding conversion technologies become a focal point. In this context, demand for electrochemical in situ characterization techniques field is gradually increasing. Understanding microscopic reactions their mechanisms depth common concern shared by both academia industry. Therefore, holds critical significance. This paper comprehensively reviews from three aspects: spectral reactions, spatial distribution optical surface refractive index associated with reactions. These characteristics are described detail, future direction technology prospected, aim promoting advancement conversion, facilitating transformation, thus advancing goals neutrality.”

Language: Английский

---