How does the defect ZnO@Au surface activate the methane via the precursor-mediated mechanism?

Liu, Guangsheng; Huang, Weiqiao; Li, Yi; Ding, Kan; Chen, Wenkai; Zhang, Yongfan; Lin, Wei

doi:10.1016/j.apsusc.2021.149728

Cited by 3 publications

(2 citation statements)

References 63 publications

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“…Oxygen vacancies induced by defect engineering on semiconducting metal oxides give rise to coordinatively unsaturated sites, which favor the chemisorption of O 2 and CH 4 . 23 In addition, constructing oxygen vacancies in metal oxides may modulate the valence band position to reduce the oxidation capacity of photogenerated holes and therefore restrain the overoxidation of CH 4 . 24 Moreover, oxygen vacancies can steer the charge carrier kinetics for enhanced photocatalysis.…”

Section: Introductionmentioning

confidence: 99%

Simultaneously Accelerating Carrier Transfer and Enhancing O₂/CH₄ Activation via Tailoring the Oxygen-Vacancy-Rich Surface Layer for Cocatalyst-Free Selective Photocatalytic CH₄ Conversion

Luo

Zhou

et al. 2022

ACS Appl. Mater. Interfaces

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Solar energy-driven direct CH4 conversion to liquid oxygenates provides a promising avenue toward green and sustainable CH4 industry, yet still confronts issues of low selectivity toward single oxygenate and use of noble-metal cocatalysts. Herein, for the first time, we report a defect-engineering strategy that rationally regulates the defective layer over TiO2 for selective aerobic photocatalytic CH4 conversion to HCHO without using noble-metal cocatalysts. (Photo)electrochemical and in situ EPR/Raman spectroscopic measurements reveal that an optimized oxygen-vacancy-rich surface disorder layer with a thickness of 1.37 nm can simultaneously promote the separation and migration of photogenerated charge carriers and enhance the activation of O2 and CH4, respectively, to •OH and •CH3 radicals, thereby synergistically boosting HCHO production in aerobic photocatalytic CH4 conversion. As a result, a HCHO production rate up to 3.16 mmol g–1 h–1 with 81.2% selectivity is achieved, outperforming those of the reported state-of-the-art photocatalytic systems. This work sheds light on the mechanism of O2-participated photocatalytic CH4 conversion on defective metal oxides and expands the application of defect engineering in designing low-cost and efficient photocatalysts.

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Section: Introductionmentioning

confidence: 99%

Simultaneously Accelerating Carrier Transfer and Enhancing O₂/CH₄ Activation via Tailoring the Oxygen-Vacancy-Rich Surface Layer for Cocatalyst-Free Selective Photocatalytic CH₄ Conversion

Luo

Zhou

et al. 2022

ACS Appl. Mater. Interfaces

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“…An appropriate concentration of defects can effectively improve the ability of the catalyst surface to activate reactant molecules (methane and oxygen molecular). For example, vacancy defects have unsaturated coordination, which is more advantageous to the adsorption of methane and the activation of C-H. 87 Liu et al 120 researched the activation mechanism for the dissociation of methane adsorbed on the triangular defect surface of ZnO@Au by DFT calculations (surface model is shown in Fig. 6D, simulating the triangular defects reported in the literature).…”

Section: Promoting the Activation Of Reactant Molecules On The Catalystsmentioning

confidence: 99%

Advancement of modification engineering in lean methane combustion catalysts based on defect chemistry

Qiu

Wang

et al. 2023

Catal. Sci. Technol.

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Single-atom catalysts in methane chemistry

Kolesnichenko,

Ezhova,

Snatenkova

2023

RUSS CHEM REV

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Обобщены и систематизированы литературные данные (с акцентом на результаты, опубликованные в последние годы), касающиеся применения в химии метана "одноатомных" катализаторов—гетерогенных каталитических контактов последнего поколения с активными металлическими центрами в виде одиночных атомов, закрепленными на подложке из неорганического материала. Рассмотрены особенности активации молекулы CH4 на поверхности таких катализаторов, проведено сравнение их поведения с поведением других известных гетерогенно-каталитических контактов, содержащих металлические нанокластеры или наночастицы активного металла, в процессах прямой окислительной и неокислительной конверсии метана в различные химические соединения. Проанализирована эффективность применения "одноатомных" катализаторов разного состава и разных модификаций (нанесенные одиночные металлические атомы, моно- и полиметаллические "одноатомные" контакты, системы сложного дисперсного состава и др.) в таких реакциях с участием метана, как сухой, паровой, окислительный риформинг, парциальное окисление в метанол, окислительное карбонилирование и карбоксилирование в уксусную кислоту, неокислительная и окислительная конденсация метана в этан(этилен), дегидроароматизация CH4, метилирование метаном бензола. Обсуждены новые возможности, открывающиеся в химии метана при использовании "одноатомных" катализаторов. Библиография —307 ссылок

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How does the defect ZnO@Au surface activate the methane via the precursor-mediated mechanism?

Cited by 3 publications

References 63 publications

Simultaneously Accelerating Carrier Transfer and Enhancing O₂/CH₄ Activation via Tailoring the Oxygen-Vacancy-Rich Surface Layer for Cocatalyst-Free Selective Photocatalytic CH₄ Conversion

Simultaneously Accelerating Carrier Transfer and Enhancing O₂/CH₄ Activation via Tailoring the Oxygen-Vacancy-Rich Surface Layer for Cocatalyst-Free Selective Photocatalytic CH₄ Conversion

Advancement of modification engineering in lean methane combustion catalysts based on defect chemistry

Single-atom catalysts in methane chemistry

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How does the defect ZnO@Au surface activate the methane via the precursor-mediated mechanism?

Cited by 3 publications

References 63 publications

Simultaneously Accelerating Carrier Transfer and Enhancing O2/CH4 Activation via Tailoring the Oxygen-Vacancy-Rich Surface Layer for Cocatalyst-Free Selective Photocatalytic CH4 Conversion

Simultaneously Accelerating Carrier Transfer and Enhancing O2/CH4 Activation via Tailoring the Oxygen-Vacancy-Rich Surface Layer for Cocatalyst-Free Selective Photocatalytic CH4 Conversion

Advancement of modification engineering in lean methane combustion catalysts based on defect chemistry

Single-atom catalysts in methane chemistry

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Product

Resources

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Simultaneously Accelerating Carrier Transfer and Enhancing O₂/CH₄ Activation via Tailoring the Oxygen-Vacancy-Rich Surface Layer for Cocatalyst-Free Selective Photocatalytic CH₄ Conversion

Simultaneously Accelerating Carrier Transfer and Enhancing O₂/CH₄ Activation via Tailoring the Oxygen-Vacancy-Rich Surface Layer for Cocatalyst-Free Selective Photocatalytic CH₄ Conversion