Designing a Built-In Electric Field for Efficient Energy Electrocatalysis

ACS Nano, Journal Year: 2022, Volume and Issue: 16(12), P. 19959 - 19979

Published: Dec. 15, 2022

To utilize intermittent renewable energy as well achieve the goals of peak carbon dioxide emissions and neutrality, various electrocatalytic devices have been developed. However, reactions, e.g., hydrogen evolution reaction/oxygen reaction in overall water splitting, polysulfide conversion lithium–sulfur batteries, formation/decomposition lithium peroxide lithium–oxygen nitrate reduction to degrade sewage, suffer from sluggish kinetics caused by multielectron transfer processes. Owing merits accelerated charge transport, optimized adsorption/desorption intermediates, raised conductivity, regulation microenvironment, ease combine with geometric characteristics, built-in electric field (BIEF) is expected overcome above problems. Here, we give a Review about very recent progress BIEF for efficient electrocatalysis. First, construction strategies characterization methods (qualitative quantitative analysis) are summarized. Then, up-to-date overviews engineering electrocatalysis, attention on electron structure optimization microenvironment modulation, analyzed discussed detail. In end, challenges perspectives proposed. This gives deep understanding design electrocatalysts next-generation storage devices.

Language: Английский

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Sustainable zinc–air battery chemistry: advances, challenges and prospects

Chemical Society Reviews, Journal Year: 2023, Volume and Issue: 52(17), P. 6139 - 6190

Published: Jan. 1, 2023

Sustainable zinc-air batteries (ZABs) are considered promising energy storage devices owing to their inherent safety, high density, wide operating temperature window, environmental friendliness, etc., showing great prospect for future large-scale applications. Thus, tremendous efforts have been devoted addressing the critical challenges associated with sustainable ZABs, aiming significantly improve efficiency and prolong operation lifespan. The growing interest in ZABs requires in-depth research on oxygen electrocatalysts, electrolytes, Zn anodes, which not systematically reviewed date. In this review, fundamentals of electrocatalysts air cathodes, physicochemical properties ZAB issues strategies stabilization anodes summarized from perspective fundamental characteristics design principles. Meanwhile, significant advances situ/operando characterization highlighted provide insights into reaction mechanism dynamic evolution electrolyte|electrode interface. Finally, several thoughts perspectives provided regarding opportunities ZABs. Therefore, review provides a thorough understanding advanced chemistry, hoping that timely comprehensive can shed light upcoming horizons prosperous area.

Language: Английский

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Microenvironment Engineering of Single/Dual‐Atom Catalysts for Electrocatalytic Application

Advanced Materials, Journal Year: 2023, Volume and Issue: 35(31)

Published: Feb. 23, 2023

Single/dual-metal atoms supported on carbon matrix can be modulated by coordination structure and neighboring active sites. Precisely designing the geometric electronic uncovering structure-property relationships of single/dual-metal confront with grand challenges. Herein, this review summarizes latest progress in microenvironment engineering single/dual-atom sites via a comprehensive comparison single-atom catalyst (SACs) dual-atom catalysts (DACs) term design principles, modulation strategy, theoretical understanding structure-performance correlations. Subsequently, recent advances several typical electrocatalysis process are discussed to get general reaction mechanisms finely-tuned SACs DACs. Finally, full-scaled summaries challenges prospects given for This will provide new inspiration development atomically dispersed electrocatalytic application.

Language: Английский

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Chemically bonded Mn0.5Cd0.5S/BiOBr S-scheme photocatalyst with rich oxygen vacancies for improved photocatalytic decontamination performance

Advanced Powder Materials, Journal Year: 2024, Volume and Issue: 3(3), P. 100183 - 100183

Published: Feb. 20, 2024

Devising exceptional S-scheme heterojunction photocatalysts utilized in annihilating pharmaceuticals and chromium contamination is significant for addressing the problem of global water pollution. In this work, a chemically bonded Mn0.5Cd0.5S/BiOBr heterostructure with oxygen vacancies ingeniously developed through facile in-situ solvothermal synthesis. The designed exhibits eminently reinforced photo-activity destruction tetracycline hydrochloride Cr (VI) as compared its individual components. This substantial photo-redox performance amelioration benefitted from creation an intense internal electric field (IEF) via supplying powerful driving force migration highway by interfacial chemical bond to foster electron/hole disintegration. More intriguingly, IEF at hetero-interface drives fast consumption photo-induced holes Mn0.5Cd0.5S photoelectrons BiOBr, profoundly boosting enrichment active photo-carriers sparing photo-corrosion Mn0.5Cd0.5S. Furthermore, anti-interference property can work efficiently real matrices. Multiple uses recycled Mn0·5Cd0·5S/BiOBr evidence prominent robustness stability. achievement indicates vast potential photosystems structural defects design photo-responsive materials effective wastewater treatment.

Language: Английский

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Tunable Interfacial Charge Transfer in a 2D–2D Composite for Efficient Visible‐Light‐Driven CO₂ Conversion

Advanced Materials, Journal Year: 2023, Volume and Issue: 35(26)

Published: March 25, 2023

Photocatalytic CO2 conversion for hydrocarbon fuel production has been known as one of the most promising strategies achieving carbon neutrality. Yet, its efficiency remains unsatisfactory mainly due to severe charge-transfer resistance and slow charge kinetics. Herein, a tunable interfacial transfer on an oxygen-vacancies-modified bismuth molybdate nanoflower assembled by 2D nanosheets (BMOVs) bismuthene composite (Bi/BMOVs) is demonstrated photocatalytic conversion. Specifically, meticulous design Ohmic contact formed between BMOVs can allow modulation resistance. According density functional theory (DFT) simulations, it ascertained that such exceptional kinetics attributed built-in electric field (IEF) contact. As such, reduction performance optimized Bi/BMOVs (CO CH4 productions rate 169.93 4.65 µmol g-1 h-1 , respectively) ca. 10 times higher than pristine BMO rates 16.06 0.51 respectively). The reported in this work shed some important light highly efficient photocatalysts both energy environmental applications.

Language: Английский

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P‐Mediated Cu–N₄ Sites in Carbon Nitride Realizing CO₂ Photoreduction to C₂H₄ with Selectivity Modulation

Advanced Materials, Journal Year: 2022, Volume and Issue: 35(3)

Published: Nov. 4, 2022

Photocatalytic CO2 reduction to high value-added C2 products (e.g., H4 ) is of considerable interest but challenging. The product selectivity strongly hinges on the intermediate energy levels in pathway. Herein, Cu-N4 sites anchored phosphorus-modulated carbon nitride (CuACs/PCN) designed as a photocatalyst tailor formation reaction pathway for realizing its production with tunable selectivity. Theoretical calculations combined experimental data demonstrate that C-C coupling intermediates can be realized and surrounding doped P facilitates . Thus, CuACs/PCN exhibits 53.2% yielding rate 30.51 µmol g-1 findings reveal significant role coordination environment microenvironment Cu single atoms offer an effective approach highly selective photoreduction produce

Language: Английский

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Atomically Dispersed Zincophilic Sites in N,P-Codoped Carbon Macroporous Fibers Enable Efficient Zn Metal Anodes

Journal of the American Chemical Society, Journal Year: 2023, Volume and Issue: 145(22), P. 12333 - 12341

Published: May 26, 2023

Zn dendrite growth and undesired parasitic reactions severely restrict the practical use of deep-cycling metal anodes (ZMAs). Herein, we demonstrate an elaborate design atomically dispersed Cu sites anchored on N,P-codoped carbon macroporous fibers (denoted as Cu/Zn-N/P-CMFs) a three-dimensional (3D) versatile host for efficient ZMAs in mildly acidic electrolyte. The 3D frameworks can alleviate structural stress suppress by spatially homogenizing Zn2+ flux. Moreover, well-dispersed atoms N P maximize utilization abundant active nucleation plating. As expected, Cu/Zn-N/P-CMFs presents low overpotential, high reversibility, dendrite-free deposition. Cu/Zn-N/P-CMFs-Zn electrode exhibits stable plating/stripping with polarization 630 h at 2 mA cm-2 mAh cm-2. When coupled MnO2 cathode, fabricated full cell also shows impressive cycling performance even when tested under harsh conditions.

Language: Английский

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Dual-Defective Two-Dimensional/Two-Dimensional Z-Scheme Heterojunctions for CO₂ Reduction

ACS Catalysis, Journal Year: 2023, Volume and Issue: 13(11), P. 7221 - 7229

Published: May 15, 2023

The target of photocatalytic CO2 reduction is to achieve high selectivity, efficiency, and stability for a single chemical/fuel production. construction conventional Z-scheme heterojunctions beneficial improve the interfacial charge separation redox capacities. However, random dimensions junction component(s) undermine charge-to-surface transport catalytic reactions, limited chemical structures catalysts restrict surface activity/selectivity tailoring. In this work, we successfully overcome these issues by stacking/constructing an ultrathin dual-defective two-dimensional (2D)/2D heterojunction with growing functional anionic vacancies onto both reductive oxidative components Z-scheme. O-vacancy-rich BiOCl/N-vacancy-rich g-C3N4-based 2D exhibits excellent photoactivity in reduction. rate photoreduction CO around 45.33 μmol g–1 h–1, which 11.7- 12.2-fold those untreated bulk g-C3N4 pristine BiOCl, respectively. Among them, N-vacancy-rich active selective ability, accompanied oxidation reactions from BiOCl. Such defective Z-schemes not only retain their original features, i.e., enhanced capacities, but also extend lower energy photon absorption ameliorate two components. Besides, density theory calculations unveiled thermodynamically favored CO2-to-CO path barrier's stepwise at COOH-to-CO rate-limiting step component further This work provides effective adaptable dual-defect engineering on 2D/2D enhance photoreduction.

Language: Английский

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Potassium and Sulfur Dual Sites on Highly Crystalline Carbon Nitride for Photocatalytic Biorefinery and CO₂ Reduction

ACS Catalysis, Journal Year: 2023, Volume and Issue: 13(3), P. 2106 - 2117

Published: Jan. 24, 2023

The co-production of high-value-added chemicals and fuels by coupling biomass photooxidation with carbon dioxide (CO2) photoreduction has attracted wide interest. Nevertheless, there still lacks comprehensive studies. Herein, we synthesized a highly crystalline nitride potassium sulfur dual sites (K/S@CN-x) salt-template-assisted incorporation method. K/S high crystallinity resulted in the photocatalytic performance significantly enhancing visible-light absorption accelerated photogenerated charge separation/transfer. Thus, K/[email protected], monoxide (CO) evolution rate (16.27 μmol g–1 h–1) lactic acid yield (78.07%) were 4.80 times 1.15 times, respectively, those CN. Furthermore, density functional theory calculations performed to investigate role K S reactions. Our findings provide unique routes for synthesizing photocatalysts demonstrate feasibility selective oxidation coupled CO2 reduction.

Language: Английский

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Ambient Electrosynthesis toward Single‐Atom Sites for Electrocatalytic Green Hydrogen Cycling

Advanced Materials, Journal Year: 2023, Volume and Issue: 35(14)

Published: Feb. 17, 2023

With the ultimate atomic utilization, well-defined configuration of active sites and unique electronic properties, catalysts with single-atom (SASs) exhibit appealing performance for electrocatalytic green hydrogen generation from water splitting further utilization via hydrogen-oxygen fuel cells, such that a vast majority synthetic strategies toward SAS-based (SASCs) are exploited. In particular, room-temperature electrosynthesis under atmospheric pressure offers novel, safe, effective route to access SASs. Herein, recent progress in ambient SASs sustainable future opportunities discussed. A systematic summary is started on three kinds electrochemically routes SASs, including electrochemical etching (ECE), direct electrodeposition (DED), leaching-redeposition (ELR), associated advanced characterization techniques. Next, their applications energy conversion evolution reaction, oxygen overall splitting, reduction reaction reviewed. Finally, brief conclusion remarks challenges regarding development high-performance cost-effective SASCs many other presented.

Language: Английский

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