p–d Orbital Hybridization Induced by p-Block Metal-Doped Cu Promotes the Formation of C₂₊ Products in Ampere-Level CO₂ Electroreduction

Journal of the American Chemical Society, Journal Year: 2023, Volume and Issue: 145(8), P. 4675 - 4682

Published: Feb. 17, 2023

Large-current electrolysis of CO2 to multi-carbon (C2+) products is critical realize the industrial application conversion. However, poor binding strength *CO intermediates on catalyst surface induces multiple competing pathways, which hinder C2+ production. Herein, we report that p-d orbital hybridization induced by Ga-doped Cu (CuGa) could promote efficient electrocatalysis at ampere-level current density. It was found CuGa exhibited highest productivity with a remarkable Faradaic efficiency (FE) 81.5% density 0.9 A/cm2, and potential such high -1.07 V versus reversible hydrogen electrode. At 1.1 still maintained an FE 76.9%. Experimental theoretical studies indicated excellent performance results from Ga, not only enriches reactive sites but also enhances intermediate facilitates C-C coupling. The strategy can be extended other p-block metal-doped catalysts, as CuAl CuGe, boost electroreduction for As far know, this first work electrochemical reduction reaction generate product interaction using catalyst.

Language: Английский

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A rational design of functional porous frameworks for electrocatalytic CO₂reduction reaction

Chemical Society Reviews, Journal Year: 2023, Volume and Issue: 52(4), P. 1382 - 1427

Published: Jan. 1, 2023

Rational design of functional porous frameworks for electrocatalytic CO 2 reduction reaction.

Language: Английский

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Modulating the microenvironment of single atom catalysts with tailored activity to benchmark the CO2 reduction

Materials Today, Journal Year: 2023, Volume and Issue: 67, P. 203 - 228

Published: June 19, 2023

Language: Английский

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Dual-site catalysts featuring platinum-group-metal atoms on copper shapes boost hydrocarbon formations in electrocatalytic CO2 reduction

Nature Communications, Journal Year: 2023, Volume and Issue: 14(1)

Published: May 27, 2023

Copper-based catalyst is uniquely positioned to catalyze the hydrocarbon formations through electrochemical CO2 reduction. The design freedom limited for alloying copper with H-affinitive elements represented by platinum group metals because latter would easily drive hydrogen evolution reaction override We report an adept of anchoring atomically dispersed metal species on both polycrystalline and shape-controlled Cu catalysts, which now promote targeted reduction while frustrating undesired reaction. Notably, alloys similar formulations but comprising small or palladium clusters fail this objective. With appreciable amount CO-Pd1 moieties surfaces, facile CO* hydrogenation CHO* CO-CHO* coupling viable as one main pathways Cu(111) Cu(100) selectively produce CH4 C2H4 Pd-Cu dual-site pathways. work broadens choices in aqueous phases.

Language: Английский

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Decorating Thermodynamically Stable (101) Facets of TiO₂ with MoO₃ for Multifunctional Sustainable Hydrogen Energy and Ammonia Gas Sensing Applications

Inorganic Chemistry, Journal Year: 2023, Volume and Issue: 63(1), P. 304 - 315

Published: Dec. 26, 2023

The simultaneous realization of sustainable energy and gas sensors dealing with the emission pollutants is indispensable as former thrives on minimization latter. However, there a dearth multifunctional nanocatalysts in literature. This ascertains importance semiconductors which can be utilized H2 generation via overall water splitting sensing global such NH3. MoO3-decorated TiO2 Z-scheme heterostructures exceptionally escalate photochemical photo/electrochemical evolution performance response owing to synergistic relationship between MoO3. Extensive structural, morphological, optical characterizations, theoretical studies, XPS results were exploited develop mechanistic framework evolution. optimum TiO2–MoO3 composition (20 wt % MoO3–TiO2) was found nearly 12- 20-fold superior pristine MoO3 photocatalysts, respectively, remarkable rate 9.18 mmol/g/h AQY 36.02%. In addition, 20 MoO3–TiO2 also showed advanced efficiency 0.61/0.7 V overpotential values toward HER due higher electrochemically active surface area Tafel slope low 65 mV/dec. NH3 turned out 2.5-fold than that sensor.

Language: Английский

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Ultrafast Microwave Synthesis of Ru-Doped MoP with Abundant P Vacancies as the Electrocatalyst for Hydrogen Generation in a Wide pH Range

Inorganic Chemistry, Journal Year: 2023, Volume and Issue: 62(24), P. 9687 - 9694

Published: June 2, 2023

Molybdenum phosphide (MoP) has received increasing attention for the hydrogen evolution reaction (HER) due to its Pt-like electronic structure and high electrical conductivity. In this work, a flake-like Ru-doped MoP with phosphorus vacancy (Ru-MoP-PV) electrocatalyst is synthesized first time by simple rapid room-temperature microwave approach within 30 s. The created abundant vacancies provide rich active sites favor electron transfer. introduced Ru also enhances catalytic activity of efficiently. Then, designed Ru-MoP-PV possesses low overpotentials HER 79, 100, 161 mV in 1.0 M KOH, 0.5 H2SO4, phosphate-buffered saline obtain 10 mA cm-2. NiFe-layered double hydroxide are used as cathode anode, respectively, drive water splitting just need cell voltage 1.6 V achieve This work provides feasible way production metal phosphides energy conversion storage applications.

Language: Английский

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Facile fabrication of polypyrrole/NiO_x core‐shell nanocomposites for hydrogen production from wastewater

Polymers for Advanced Technologies, Journal Year: 2023, Volume and Issue: 34(5), P. 1633 - 1641

Published: Feb. 2, 2023

Abstract This work highlights testing the polymer nanocomposite for hydrogen gas production from wastewater (sewage water). The in‐situ polymerization technique is used to prepare polypyrrole (PPy) and PPy/NiO x films on a glass substrate. film's ability generate sewage water then evaluated. XRD XPS confirmed formation of two types NiO X : Ni 2 O 3 . optical property composite greater than under insertion as core coating shell, in which band gap values are 2.25 1.81 eV, respectively. TEM core‐shell formation, shell (20 nm) coated (170 nm). electrochemical H carried out through three‐electrode cell. effect light on/off, wavelengths, temperature applied. Under off/on light, produced current density ( J ph ) value enhanced 5 16 μA, monochromatic light: 440, 540, 730 nm tested, −1.28, −1.16, −1.14 μA cm −2 , In which, decreasing with increasing behavior photoelectrode different regions. increase −1.6 −5.8 rise 30 55°C. Moreover, enthalpy (Δ *), activation energy E ), entropy S *) thermodynamic processes determined using response at temperatures.

Language: Английский

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Electronic modulation of a single-atom-based tandem catalyst boosts CO₂ photoreduction to ethanol

Energy & Environmental Science, Journal Year: 2023, Volume and Issue: 16(12), P. 5956 - 5969

Published: Jan. 1, 2023

A single-atom-based tandem photocatalyst (In 2 O 3 /Cu–O ) is fabricated for efficient CO -to-ethanol conversion. The electronic interaction between Cu and In promotes C–C coupling of *CO (on site) *COH Cu–O to form OC–COH species.

Language: Английский

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Palladium-Copper bimetallic catalysts for electroreduction of CO2 and nitrogenous species

Coordination Chemistry Reviews, Journal Year: 2024, Volume and Issue: 509, P. 215802 - 215802

Published: March 26, 2024

Language: Английский

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MoS₂-Based Nanocomposites for Photocatalytic Hydrogen Evolution and Carbon Dioxide Reduction

ACS Omega, Journal Year: 2023, Volume and Issue: 8(29), P. 25649 - 25673

Published: July 12, 2023

Photocatalysis is a facile and sustainable approach for energy conversion environmental remediation by generating solar fuels from water splitting. Due to their two-dimensional (2D) layered structure excellent physicochemical properties, molybdenum disulfide (MoS2) has been effectively utilized in photocatalytic H2 evolution reaction (HER) CO2 reduction. The efficiency of MoS2 greatly depends on the active edge sites present structure. Modifications like reducing layer numbers, creating defective structures, adopting different morphologies produce more unsaturated S atoms as sites. Hence, acts cocatalyst nanocomposites/heterojunctions facilitate photogenerated electron transfer. This review highlights role nanocomposites activity described comprehensively binary (with metal oxide, carbonaceous materials, sulfides, metal-organic frameworks) ternary composites MoS2. Photocatalytic reduction complex challenging process that demands an efficient light-responsive semiconductor catalyst tackle thermodynamic kinetic factors. using emerging topic would be cost-effective substitute noble catalysts. Herein, we also exclusively envisioned possibility its this area. expected furnish understanding diverse roles fuel generation, thus endorsing interest utilizing unique create nanostructures future applications.

Language: Английский

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