Dual Active Sites Decorated Tungsten Trioxide for Photocatalytic Methane Oxidation DOI
Shan Shan Qiu, Xiaoxin Liu, Jiacheng Liang

et al.

Advanced Energy Materials, Journal Year: 2025, Volume and Issue: unknown

Published: April 16, 2025

Abstract Photocatalytic oxidation of methane to formaldehyde offers an appealing pathway for utilizing the abundant resource, nevertheless, suffering from poor formation rate and selectivity. Here, nickel cluster decorated tungsten trioxide three high surface energy facets is prepared photocatalytic with yield 3.27 mmol g −1 h , selectivity 98.2% turnover number 20.65. The dual photohole centers lattice oxygen both could activate selective formation. involves whole process on catalyst based active site mechanism, while promotes methyl radical facilitates a mechanism in aqueous phase near surface. These sites provide effective strategy oxidize under photoirradiation water gas.

Language: Английский

Catalyzing Artificial Photosynthesis with TiO2 Heterostructures and Hybrids: Emerging Trends in a Classical yet Contemporary Photocatalyst DOI Open Access
Xiaowen Ruan, Shijie Li,

Chengxiang Huang

et al.

Advanced Materials, Journal Year: 2023, Volume and Issue: 36(17)

Published: Oct. 11, 2023

Titanium dioxide (TiO

Citations

71
Light-driven flow synthesis of acetic acid from methane with chemical looping DOI Creative Commons
Wenqing Zhang, Dawei Xi, Yihong Chen

et al.

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

Published: May 26, 2023

Oxidative carbonylation of methane is an appealing approach to the synthesis acetic acid but limited by demand for additional reagents. Here, we report a direct CH3COOH solely from CH4 via photochemical conversion without This made possible through construction PdO/Pd-WO3 heterointerface nanocomposite containing active sites activation and C-C coupling. In situ characterizations reveal that dissociated into methyl groups on Pd while oxygen PdO responsible carbonyl formation. The cascade reaction between generates acetyl precursor which subsequently converted CH3COOH. Remarkably, production rate 1.5 mmol gPd-1 h-1 selectivity 91.6% toward achieved in flow reactor. work provides insights intermediate control material design, opens avenue oxygenates.

Language: Английский

Citations

52
Photodriven Methane Conversion on Transition Metal Oxide Catalyst: Recent Progress and Prospects DOI Creative Commons
Pu Wang, Run Shi, Jiaqi Zhao

et al.

Advanced Science, Journal Year: 2023, Volume and Issue: 11(8)

Published: Oct. 26, 2023

Methane as the main component in natural gas is a promising chemical raw material for synthesizing value-added chemicals, but its harsh conversion process often causes severe energy and environment concerns. Photocatalysis provides an attractive path to active convert methane into various products under mild conditions with clean sustainable solar energy, although many challenges remain at present. In this review, recent advances photocatalytic are systematically summarized. As basis of conversion, activation first elucidated from structural molecules. The study committed categorizing elucidating research progress laws intricate reactions according target products, including partial oxidation, reforming, coupling, combustion, functionalization. Advanced reactor designs also designed enrich options reliability performance evaluation. prospects discussed, which turn offers guidelines methane-conversion-related photocatalyst exploration, reaction mechanism investigation, advanced photoreactor design.

Language: Английский

Citations

43
Heterogeneous Photocatalytic Strategies for C(sp3)−H Activation DOI Creative Commons
Zhigang Chai

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(13)

Published: Jan. 16, 2024

Abstract Activation of ubiquitous C(sp 3 )−H bonds is extremely attractive but remains a great challenge. Heterogeneous photocatalysis offers promising and sustainable approach for activation has been fast developing in the past decade. This Minireview focuses on mechanism strategies heterogeneous photocatalytic activation. After introducing mechanistic insights, including precise design active sites, regulation reactive radical species, improving charge separation reactor innovations are discussed. In addition, recent advances hydrocarbons, alcohols, ethers, amines amides by summarized. Lastly, challenges opportunities outlined to encourage more efforts development this exciting field.

Language: Английский

Citations

17
Best Practices for Experiments and Reports in Photocatalytic Methane Conversion DOI
Yuheng Jiang, Siyang Li, Yingying Fan

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(24)

Published: April 4, 2024

Efficiently converting methane into valuable chemicals via photocatalysis under mild condition represents a sustainable route to energy storage and value-added manufacture. Despite continued interest in this area, the achievements have been overshadowed by absence of standardized protocols for conducting photocatalytic oxidation experiments as well evaluating corresponding performance. In review, we present structured solution aimed at addressing these challenges. Firstly, introduce norms underlying reactor design outline various configurations gas-solid gas-solid-liquid reaction systems. This discussion helps choosing suitable reactors conversion experiments. Subsequently, offer comprehensive step-by-step protocol applicable diverse methane-conversion reactions. Emphasizing meticulous verification accurate quantification products, highlights significance mitigating contamination sources selecting appropriate detection methods. Lastly, propose performance metrics crucial conversion. By defining metrics, community could obtain consensus assessing across different studies. Moving forward, future necessitates further refinement stringent experimental standards evaluation criteria. Moreover, development scalable is essential facilitate transition from laboratory proof-of-concept potentially industrial production.

Language: Английский

Citations

17
Sustainable Energy Resources for Driving Methane Conversion DOI
Rong Chen, Guo‐Ming Weng

Advanced Energy Materials, Journal Year: 2023, Volume and Issue: 13(36)

Published: Aug. 13, 2023

Abstract The conversion of methane to value‐added chemicals by traditional reforming processes suffers from intensive energy consumption due its particularly strong C─H bonds. Thus, it is urgent optimize the driving force structure for accelerating integration sustainable energy. In this review, advances in energy‐driven are systematically summarized provide a scientific understanding operation/storage concepts, reactor design, technological maturity, system optimization, and remaining issues. Furthermore, essence, economic evaluations, balance, social impacts driven carefully discussed, paving path future course research development. Diversifying mix can play an important role industries, being used as crucial step transition energy, especially combination solar/nuclear with fossil fuels produce chemicals. Additionally, review intends bridge studies development, ultimate goal offering robust framework understand current status guidance design solutions greener future.

Language: Английский

Citations

31
Interstitial Zinc Defects Enriched ZnO Tuning O2 Adsorption and Conversion Pathway for Superior Photocatalytic CH4 Oxygenation DOI
Zhen Xiao, Zhenyu Wan,

Jiangjie Zhang

et al.

ACS Catalysis, Journal Year: 2024, Volume and Issue: 14(12), P. 9104 - 9114

Published: May 30, 2024

Photocatalytic methane conversion into liquid oxygenates using O2 oxidants provides a promising approach for high-value chemicals. The generation of reactive oxygen species and their reaction pathway are key to determine the oxygenate selectivity. Here, an interstitial Zni defect ZnO (ZnO(Zni)) is developed through thermal decomposition ZnO2 precursor. favors adsorption at terminal configuration induces effectively desired •OOH instead •OH improving yield selectivity oxygenates. For comparison, adsorbed in lateral tends be converted excessive on typical Au/ZnO. As result, ZnO(Zni) shows 6080 μmol g–1 with 98.6% selectivity, which leads 10 times lower than Au/ZnO CO2 release overoxidation. This work activation regulate photocatalytic CH4 oxidation

Language: Английский

Citations

14
Boosting Gas-Phase TiO2 Photocatalysis with Weak Electric Field Strengths of Volt/Centimeter DOI

My Nghe Tran,

Myriam Moreau, Ahmed Addad

et al.

ACS Applied Materials & Interfaces, Journal Year: 2024, Volume and Issue: 16(12), P. 14852 - 14863

Published: March 19, 2024

Among semiconductor nanomaterials, titanium dioxide is at the forefront of heterogeneous photocatalysis, but its catalytic activity greatly suffers from loss photoexcited charge carriers through deleterious recombination processes. Here, we investigate impact an external electric field (EEF) applied to conventional P25 TiO

Language: Английский

Citations

12
Nitrogen-Doped Titanium Dioxide for Selective Photocatalytic Oxidation of Methane to Oxygenates DOI
Guanghui Feng, Jianing Mao, Tong Sun

et al.

ACS Applied Materials & Interfaces, Journal Year: 2024, Volume and Issue: 16(4), P. 4600 - 4605

Published: Jan. 19, 2024

Photocatalytic conversion of methane (CH4) to value-added chemicals using H2O as the oxidant under mild conditions is a desired sustainable pathway for synthesizing commodity chemicals. However, controlling product selectivity while maintaining high yields greatly challenging. Herein, we develop highly efficient strategy, based on precise control types nitrogen dopants, and design photocatalysts, achieve productivity oxygenates via CH4 photocatalytic conversion. The primary (methanol) obtained in yield 159.8 μmol·g–1·h–1 47.7% selectivity, oxygenate compounds reached 92.5%. unique hollow porous structure substituted sites nitrogen-doped TiO2 synergistically promote its photo-oxidation performance. Furthermore, situ attenuated total reflectance Fourier transform infrared spectroscopy provides direct evidence key intermediates their evolution producing methanol multicarbon oxygenates. This study insights into mechanism

Language: Английский

Citations

10
Single‐cluster Functionalized TiO2 Nanotube Array for Boosting Water Oxidation and CO2 Photoreduction to CH3OH DOI

Shen‐Yue Xu,

Wenxiong Shi, Juanru Huang

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(28)

Published: April 26, 2024

Abstract Solar‐driven CO 2 reduction and water oxidation to liquid fuels represents a promising solution alleviate energy crisis climate issue, but it remains great challenge for generating CH 3 OH dominated by multi‐electron transfer. Single‐cluster catalysts with super electron acceptance, accurate molecular structure, customizable electronic structure multiple adsorption sites, have led greater potential in catalyzing various challenging reactions. However, accurately controlling the number arrangement of clusters on functional supports still faces challenge. Herein, we develop facile electrosynthesis method uniformly disperse Wells‐Dawson‐ Keggin‐type polyoxometalates TiO nanotube arrays, resulting series single‐cluster functionalized P M 18 O 62 @TiO PM 12 40 (M=Mo or W). The single polyoxometalate cluster can be distinctly identified serves as sponge accept electrons from excited enhancing surface‐hole concentration promote oxidation. Among these samples, Mo ‐1 exhibits highest consumption rate 1260 μmol g −1 ‐to‐CH conversion H source, which is 11 times higher than that isolated arrays. This work supplied simple synthesis realize single‐dispersion enrich surface‐reaching holes , thereby facilitating reduction.

Language: Английский

Citations

8