Single-atom catalysts for photocatalytic energy conversion

Joule, Год журнала: 2022, Номер 6(1), С. 92 - 133

Опубликована: Янв. 1, 2022

Artificial photocatalytic energy conversion represents a highly intriguing strategy for solving the crisis and environmental problems by directly harvesting solar energy. The development of efficient photocatalysts is central task pushing real-world application reactions. Due to maximum atomic utilization efficiency distinct advantages outstanding catalytic activity, single-atom catalysts (SACs) have emerged as promising candidates photocatalysts. In current review, recent progresses challenges on SACs systems are presented. Fundamental principles focusing charge separation/transfer molecular adsorption/activation photocatalysis systemically explored. We outline how isolated reactive sites facilitate photogenerated electron–hole transfer promote construction photoactivation cycles. widespread adoption in diverse reactions also comprehensively introduced. By presenting these advances addressing some future with potential solutions related integral over SACs, we expect shed light forthcoming research conversion.

Язык: Английский

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Highly Selective CO₂ Electroreduction to C₂H₄ Using a Metal–Organic Framework with Dual Active Sites

Journal of the American Chemical Society, Год журнала: 2021, Номер 143(19), С. 7242 - 7246

Опубликована: Май 6, 2021

Conversion from CO2 to C2H4 is important for the development of energy and environment, but high barrier hydrogenation *CO intermediate C–C coupling step tend result in C1 compounds as main product thus restrict generation C2H4. Here, we report a metal–organic framework (denoted PcCu-Cu-O), composed 2,3,9,10,16,17,23,24-octahydroxyphthalo-cyaninato)copper(II) (PcCu-(OH)8) ligands square-planar CuO4 nodes, electrocatalyst Compared with discrete molecular copper-phthalocyanine (Faradaic efficiency (FE) = 25%), PcCu-Cu-O exhibits much higher performance electrocatalytic reduction FE 50(1)% current density 7.3 mA cm–2 at potential −1.2 V vs RHE 0.1 M KHCO3 solution, representing best reported date. In-situ infrared spectroscopy control experiments suggested that enhanced electrochemical may be ascribed synergistic effect between CuPc unit unit, namely CO on CO-producing site (CuO4 site) can efficiently migrate dimerize adsorbed C2H4-producing (CuPc), giving lower dimerization barrier.

Язык: Английский

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Platinum Modulates Redox Properties and 5‐Hydroxymethylfurfural Adsorption Kinetics of Ni(OH)₂ for Biomass Upgrading

Angewandte Chemie International Edition, Год журнала: 2021, Номер 60(42), С. 22908 - 22914

Опубликована: Авг. 18, 2021

Abstract Nickel hydroxide (Ni(OH) 2 ) is a promising electrocatalyst for the 5‐hydroxymethylfurfural oxidation reaction (HMFOR) and dehydronated intermediates Ni(OH)O species are proved to be active sites HMFOR. In this study, Ni(OH) modified by platinum adjust electronic structure current density of HMFOR improves 8.2 times at Pt/Ni(OH) electrode compared with that on electrode. Operando methods reveal introduction Pt optimized redox property accelerate formation during catalytic process. Theoretical studies demonstrate enhanced kinetics originates from reduced dehydrogenation energy . The product analysis transition state simulation prove also reduces adsorption HMF behavior as can act site HMF. Overall, work here provides strategy design an efficient universal nickel‐based catalyst electro‐oxidation, which extended other Ni‐based catalysts such Ni(HCO 3 NiO.

Язык: Английский

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Atomically Dispersed Indium‐Copper Dual‐Metal Active Sites Promoting C−C Coupling for CO₂ Photoreduction to Ethanol

Angewandte Chemie International Edition, Год журнала: 2022, Номер 61(40)

Опубликована: Авг. 10, 2022

Photoreduction of CO2 to C2+ solar fuel is a promising carbon-neutral technology for renewable energy. This strategy challenged by its low productivity due efficiency in multielectron utilization and slow C-C coupling kinetics. work reports dual-metal photocatalyst consisting atomically dispersed indium copper anchored on polymeric carbon nitride (InCu/PCN), which the photoreduction delivered an excellent ethanol production rate 28.5 μmol g-1 h-1 with high selectivity 92 %. Coupled experimental investigation DFT calculations reveal following mechanisms underpinning performance this catalyst. Essentially, In-Cu interaction enhances charge separation accelerating transfer from PCN metal sites. Indium also transfers electrons neighboring via Cu-N-In bridges, increasing electron density active Furthermore, sites promote adsorption *CO intermediates lower energy barrier coupling.

Язык: Английский

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Engineering the Coordination Sphere of Isolated Active Sites to Explore the Intrinsic Activity in Single-Atom Catalysts

Nano-Micro Letters, Год журнала: 2021, Номер 13(1)

Опубликована: Июнь 7, 2021

Abstract Reducing the dimensions of metallic nanoparticles to isolated, single atom has attracted considerable attention in heterogeneous catalysis, because it significantly improves atomic utilization and often leads distinct catalytic performance. Through extensive research, been recognized that local coordination environment atoms an important influence on their electronic structures behaviors. In this review, we summarize a series representative systems single-atom catalysts, discussing preparation, characterization, structure–property relationship, with emphasis correlation between spheres isolated reactive centers intrinsic activities. We also share our perspectives current challenges future research promises development catalysis. With article, aim highlight possibility finely tuning performances by engineering sites provide new insights into further for emerging field.

Язык: Английский

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Co/MoC Nanoparticles Embedded in Carbon Nanoboxes as Robust Trifunctional Electrocatalysts for a Zn–Air Battery and Water Electrocatalysis

ACS Nano, Год журнала: 2021, Номер 15(8), С. 13399 - 13414

Опубликована: Авг. 4, 2021

To meet the application needs of rechargeable Zn-air battery and electrocatalytic overall water splitting (EOWS), developing high-efficiency, cost-effective, durable trifunctional catalysts for hydrogen evolution reaction (HER), oxygen evolution, reduction (OER ORR) is extremely paramount yet challenging. Herein, interface engineering concept nanoscale hollowing design were proposed to fabricate N-doping carbon nanoboxes confined with Co/MoC nanoparticles. Uniform zeolitic imidazolate framework nanocube was employed as starting material construct electrocatalyst through conformal polydopamine-Mo layer coating subsequent pyrolysis treatment. The Co@IC/MoC@PC catalyst displayed superior electrochemical ORR performances a positive half-wave potential 0.875 V high limiting current density 5.89 mA/cm2. When practically an in regenerative battery, specific capacity 728 mAh/g, large peak power 221 mW/cm2, open-circuit voltage 1.482 V, low charge/discharge gap 0.41 obtained. Moreover, its practicability further exploited by splitting, affording overpotentials 277 68 mV at 10 mA/cm2 OER HER 1 M KOH solution, respectively, decent operating 1.57 EOWS. Ultraviolet photoelectron spectroscopy functional theory calculation revealed that synergistically facilitated charge-transfer, thereby contributing enhancements ORR/OER/HER processes. More importantly, this can offer some interesting prospects construction outstanding toward various energy conversion storage devices.

Язык: Английский

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A pyrolysis-free Ni/Fe bimetallic electrocatalyst for overall water splitting

Nature Communications, Год журнала: 2023, Номер 14(1)

Опубликована: Март 31, 2023

Catalysts capable of electrochemical overall water splitting in acidic, neutral, and alkaline solution are important materials. This work develops bifunctional catalysts with single atom active sites through a pyrolysis-free route. Starting conjugated framework containing Fe sites, the addition Ni atoms is used to weaken adsorption electrochemically generated intermediates, thus leading more optimized energy level sand enhanced catalytic performance. The synthesis also ensured formation well-defined within structure, providing ideal platforms understand processes. as-prepared catalyst exhibits efficient capability for both acidic electrolytes. At current density 10 mA cm-2, overpotential hydrogen evolution oxygen 23/201 mV 42/194 0.5 M H2SO4 1 KOH, respectively. Our not only route towards applicable across wide range pH values, it provides successful showcase model in-depth mechanistic insight into splitting.

Язык: Английский

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Electrochemical reduction of carbon dioxide to multicarbon (C₂₊) products: challenges and perspectives

Energy & Environmental Science, Год журнала: 2023, Номер 16(11), С. 4714 - 4758

Опубликована: Янв. 1, 2023

This review analyzes advanced catalysts and C 2+ synthesis mechanisms based on theoretical explorations in situ / operando characterizations. Triphasic interface optimization is discussed for the potential of industry-compatible stability.

Язык: Английский

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A Review on Photothermal Conversion of Solar Energy with Nanomaterials and Nanostructures: From Fundamentals to Applications

Advanced Sustainable Systems, Год журнала: 2022, Номер 6(9)

Опубликована: Июль 6, 2022

Abstract Solar energy is a green, sustainable, and de facto inexhaustible source for mankind. The conversion of solar into other forms has attracted extensive research interest due to climate change the crisis. Among all technologies, photothermal exhibits unique advantages when applied water purification, desalination, high‐temperature heterogeneous catalysis, anti‐bacterial treatments, deicing. In this review, various mechanisms based on different heat release are summarized some latest examples presented. addition, necessary prerequisites solar‐driven materials toward their practical applications also discussed. Further, advances in discussed, focusing types applications. Finally, summary given challenges opportunities This review aims give comprehensive understanding emerging technologies effect, especially by using nanomaterials nanostructures.

Язык: Английский

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The effect of coordination environment on the activity and selectivity of single-atom catalysts

Coordination Chemistry Reviews, Год журнала: 2022, Номер 461, С. 214493 - 214493

Опубликована: Март 10, 2022

Язык: Английский

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