ACS Catalysis, Journal Year: 2025, Volume and Issue: unknown, P. 7780 - 7791
Published: April 25, 2025
Language: Английский
ACS Catalysis, Journal Year: 2025, Volume and Issue: unknown, P. 7780 - 7791
Published: April 25, 2025
Language: Английский
Energy storage materials, Journal Year: 2024, Volume and Issue: 69, P. 103429 - 103429
Published: April 23, 2024
Language: Английский
Citations
21Inorganic Chemistry Frontiers, Journal Year: 2024, Volume and Issue: 11(14), P. 4080 - 4106
Published: Jan. 1, 2024
This summary describes the effects of wettability, local pH, interfacial water structure, and electrolyte composition on interface reactant compositions, key intermediate adsorption, reaction kinetics.
Language: Английский
Citations
16Nature Communications, Journal Year: 2025, Volume and Issue: 16(1)
Published: Feb. 19, 2025
Abstract Acidic electrochemical CO 2 conversion is a promising alternative to overcome the low utilization. However, over-reliance on highly concentrated K + inhibit hydrogen evolution reaction also causes (bi)carbonate precipitation interfere with catalytic performance. In this work, under screening and guidance of computational simulations, we present carbon coated tip-like O 3 electrocatalyst for stable efficient acidic synthesize formic acid (HCOOH) concentration. The layer protects oxidized species higher intrinsic activity from reductive corrosion, peripherally formulates tip-induced electric field regulate adverse H attraction desirable enrichment. an electrolyte at pH 0.94, only 0.1 M required achieve Faradaic efficiency (FE) 98.9% 300 mA cm −2 HCOOH long-time stability over100 h. By up-scaling electrode into 25 electrolyzer setup, total current 7 A recorded sustain durable production 291.6 mmol L −1 h .
Language: Английский
Citations
2ACS Catalysis, Journal Year: 2023, Volume and Issue: 13(24), P. 16222 - 16239
Published: Dec. 5, 2023
Electric double layers form at electrode–electrolyte interfaces and often play defining roles in governing electrochemical reaction rates selectivity. While layer formation has remained an active area of research for more than a century, most frameworks used to predict electric properties, such as local ion concentrations, potential gradients, reactant chemical potentials, remain rooted classical Gouy–Chapman–Stern theory, which neglects ion–ion interactions assumes nonreactive interfaces. Yet, recent findings from the surface forces electrocatalysis communities have highlighted how emergence fundamentally alters mechanisms interface properties. Notably, studies with ionic liquids show that correlations clustering can substantially alter selectivity, especially concentrated electrolytes. Further, emerging suggest structures dynamics significantly change potentials where electrocatalytic reactions occur. Here, we provide our perspective on impact properties contribute modulating systems, under conditions high concentrations large applied cause deviations electrolyte theory. We also summarize growing questions opportunities further explore drastically conclude these open door using study achieve conversion by engineering
Language: Английский
Citations
25JACS Au, Journal Year: 2023, Volume and Issue: 3(9), P. 2336 - 2355
Published: Aug. 23, 2023
Proton exchange membrane water electrolysis (PEMWE) is the technology of choice for large-scale production green hydrogen from renewable energy. Current PEMWEs utilize large amounts critical raw materials such as iridium and platinum in anode cathode electrodes, respectively. In addition to its high cost, use Ir-based catalysts may represent a bottleneck PEM electrolyzers since very expensive, scarce, ill-distributed element. Replacing anodes challenging matter Ir-oxides are only with sufficient stability under highly oxidant environment reaction. One current strategies aiming reduce Ir content design advanced Ir-mixed oxides, which introduction cations different crystallographic sites can help engineer active certain characteristics, that is, environment, coordination, distances, oxidation state, etc. This strategy comes own problems, most mixed oxides lack during OER acidic electrolyte, suffering severe structural reconstruction, lead surfaces catalytic activity durability original oxide. Only after understanding reconstruction process would it be possible durable stable OER. this Perspective, we highlight successful electrolyte discuss promising lines evolution field.
Language: Английский
Citations
24Frontiers in Chemistry, Journal Year: 2024, Volume and Issue: 11
Published: Jan. 4, 2024
Selecting the ideal anodic potential conditions and corresponding limiting current density to generate reactive oxygen species, especially hydroxyl radical ( • OH), becomes a major challenge when venturing into advanced electrochemical oxidation processes. In this work, step-by-step guide for generation of OH on boron-doped diamond (BDD) beginners is shown, in which following steps are discussed: i) BDD activation (assuming it new), ii) response (in electrolyte ferri/ferro-cyanide), iii) Tafel plots using sampled voltammetry evaluate overpotential region where mainly generated, iv) study entrapment predominant according plots, v) finally, previously found applied degradation amoxicillin, instantaneous efficiency relative cost process reported.
Language: Английский
Citations
11Advanced Functional Materials, Journal Year: 2024, Volume and Issue: 34(45)
Published: May 28, 2024
Abstract 2D semiconductor nanomaterials have received significant attention as photocatalysts for solar‐to‐hydrogen conversion due to their robust light absorption capacity, large specific surface area, and superior electron transport characteristics. Nevertheless, it is challenging develop quaternary copper‐based sulfides (QCSs) with functional integration of conducive structural features photocatalysis from multiple elements intricate control conditions. Herein, ultrathin alloyed Cu−Ga−Zn−S (CGZS) curved nanobelts (NBs) are fabricated by using a facile one‐pot colloidal method. Subsequently, the derived Cu 31 S 16 ‐CGZS Janus heterostructures designed increasing concentrations. The formation mechanism alloys systematically investigated. Without cocatalysts, CGZS NBs demonstrated photocatalytic activities 1264.2 µmol g −1 h compared heterostructured −CGZS (463.1 ) under visible (> 400 nm). Experimental theoretical results unveiled that improved can be attributed enhanced charge–carrier separation efficiency resulting high crystallinity structure, abundant active sites high‐active (0001) crystal facet lowest reaction Gibbs energy, work function, metal‐like properties. This offers new insights into QCSs visible‐light performance.
Language: Английский
Citations
9Chemical Reviews, Journal Year: 2024, Volume and Issue: 124(22), P. 12391 - 12462
Published: Nov. 11, 2024
The electrical double layer (EDL) plays a central role in electrochemical energy systems, impacting charge transfer mechanisms and reaction rates. fundamental importance of the EDL interfacial electrochemistry has motivated researchers to develop theoretical experimental approaches assess properties. In this contribution, we review recent progress evaluating characteristics such as double-layer capacitance, highlighting some discrepancies between theory experiment discussing strategies for their reconciliation. We further discuss merits challenges various techniques having important implications aqueous electrocatalysis. A strong emphasis is placed on substantial impact electrode composition structure electrolyte chemistry addition, effects temperature pressure compare solid-liquid interfaces solid-solid interfaces.
Language: Английский
Citations
9Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: unknown
Published: Nov. 18, 2024
Electrolyte alkaline cations can significantly modulate the reaction selectivity of electrochemical CO2 reduction (eCO2R), enhancing yield valuable multicarbon (C2+) chemical feedstocks. However, mechanism underlying this cation effect on C–C coupling remains unclear. Herein, by performing constant-potential AIMD simulations, we studied dynamic behavior interfacial K+ ions over Cu surfaces during and origin effect. We showed that specific adsorption readily occurs at surface sites adjacent to *CO intermediates surfaces. Furthermore, *CO–*CO is more important than quasi-specific for kinetics, reducing barriers approximately 0.20 eV. Electronic structure analysis revealed charge redistribution between specifically adsorbed K+, *CO, sites, account reduced barriers. In addition, identified excellent Cu(100) with ions. Experimental results show suppressing K+-specific using surfactant cetyltrimethylammonium bromide (CTAB) decreases Faradaic efficiency C2 products from 41.1% 4.3%, consistent our computational findings. This study provides crucial insights improving toward C2+ rationally tuning eCO2R. Specifically, be enhanced promoting adsorption, example, confining within a coated layer or pulsed negative potentials.
Language: Английский
Citations
9Molecular Catalysis, Journal Year: 2025, Volume and Issue: 573, P. 114810 - 114810
Published: Jan. 5, 2025
Language: Английский
Citations
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