Atomically Dispersed Nickel Anchored on a Nitrogen‐Doped Carbon/TiO₂Composite for Efficient and Selective Photocatalytic CH₄Oxidation to Oxygenates

Angewandte Chemie International Edition, Год журнала: 2022, Номер 62(4)

Опубликована: Ноя. 30, 2022

Direct photocatalytic oxidation of methane to liquid oxygenated products is a sustainable strategy for valorization at room temperature. However, in this reaction, noble metals are generally needed function as cocatalysts obtaining adequate activity and selectivity. Here, we report atomically dispersed nickel anchored on nitrogen-doped carbon/TiO2 composite (Ni-NC/TiO2 ) highly active selective catalyst photooxidation CH4 C1 oxygenates with O2 the only oxidant. Ni-NC/TiO2 exhibits yield 198 μmol 4 h selectivity 93 %, exceeding that most reported high-performance photocatalysts. Experimental theoretical investigations suggest single-atom Ni-NC sites not enhance transfer photogenerated electrons from TiO2 isolated Ni atoms but also dominantly facilitate activation form key intermediate ⋅OOH radicals, which synergistically lead substantial enhancement both

Язык: Английский

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Oxygen Vacancy Defect Engineering of Heterophase Junction TiO₂: Interfacial/Surface Oxygen Vacancies Coadjust the Photocatalytic ROS Production

ACS Applied Energy Materials, Год журнала: 2022, Номер 6(2), С. 1025 - 1036

Опубликована: Дек. 30, 2022

In this study, TiO2 samples are synthesized through two stages including hydrolysis and calcination. It is found that the addition of HCl in stage could facilitate formation heterophase junction TiO2. By annealing at 300 °C an argon atmosphere, interfacial oxygen vacancies (Vo) surface Vo (distributed anatase phase) can be constructed After photocatalytic experiments, it interface have a synergistic effect production reactive species (ROSs). Surface enrich O2 transmit electrons to on anatase. Therefore, enriched converted into •O2– 1O2 easily. The not only electron transmission between phases but also change transfer mode from I-scheme Z-scheme. Thus, make photogenerated holes leave rutile. These rutile part high oxidation potential better oxidize H2O (or OH–) molecules •OH. They 1O2. This work promotes further development defect design application materials.

Язык: Английский

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Recent advances on aerobic photocatalytic methane conversion under mild conditions

Nano Research, Год журнала: 2023, Номер 16(11), С. 12558 - 12571

Опубликована: Окт. 31, 2023

Язык: Английский

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P‐N Heterojunction Embedded CuS/TiO₂ Bifunctional Photocatalyst for Synchronous Hydrogen Production and Benzylamine Conversion

Small, Год журнала: 2023, Номер 20(10)

Опубликована: Окт. 24, 2023

Abstract The coupling of photocatalytic hydrogen production and selective oxidation benzylamine is a topic significant research interest. However, enhancing the bifunctional activity in this context still major challenge. construction Z‐scheme heterojunctions an effective strategy to enhance photocatalysts. Herein, p‐n type direct heterojunction CuS/TiO 2 constructed using metal‐organic framework (MOF)‐derived TiO as substrate. carrier density measured by Mott‐Schottky under photoexcitation, which confirms that electron transfer mode driven diffusion effect caused concentration difference. Benefiting from efficient charge separation transfer, photogenerated electrons, holes are directedly transferred active reduction sites. also exhibits excellent without noble metal cocatalysts. Among them, H evolution found be 17.1 29.5 times higher than CuS, respectively. Additionally, yields N‐Benzylidenebenzylamine (NBB) 14.3 47.4 those

Язык: Английский

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Electron-Delocalization-Stabilized Photoelectrocatalytic Coupling of Methane by NiO-Polyoxometalate Sub-1 nm Heterostructures

Journal of the American Chemical Society, Год журнала: 2023, Номер 145(43), С. 23681 - 23690

Опубликована: Окт. 20, 2023

The oxidative coupling of methane to C2 oxygenates merits great scientific and technological potential yet remains a challenge due its inferior selectivity. Subnanomaterials (SNMs) with "p-n-p-n"-type heteroconstructions feature enhanced external field properties tunable electronic structures, serving as promising catalysts for the selective partial oxidation methane. Here we develop NiO-polyoxometalate (POM) subnanocoils thickness 1.8 nm, showing excellent catalytic activity toward photoelectrochemical into product under mild conditions (1 bar, 25 °C) notable productivity (up 4.48 mmol gcat-1 h-1) high selectivity (>99%). Under coupling, C-H bonds can be activated by NiO, resulted *COOH intermediates are stabilized delocalized electrons in POM clusters. contiguous active sites NiO at molecular level allow situ oxalate. This work points out an economic way may enlighten design functional SNMs from fundamental standpoints.

Язык: Английский

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