Au/Sr-ZnO双位点工程用于晶格氧活化甲烷高选择性偶联制乙烷-CSCIED科技核心评价数据库-手机版

Au/Sr-ZnO双位点工程用于晶格氧活化甲烷高选择性偶联制乙烷

Dual-site engineering of Au/Sr-ZnO photocatalysts for lattice oxygen-activated methane coupling to ethane with high selectivity

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DOI	10.1016/j.apcatb.2025.125437
刊名	Applied Catalysis B: Environment and Energy
年，卷(期)	2025, 375()
作者	王萍, 冯晓燕, 梁军 * , 张金宇, 牛涛涛, 李莉 *,
作者单位	宁夏大学
摘要	光驱动甲烷氧化偶联制乙烷是一种可持续生产高附加值化学品的前沿策略，但其C-H键断裂的高活化能垒带来显著挑战。本研究展示了一种双位点工程设计的金/锶掺杂氧化锌（Au/Sr-ZnO）光催化剂，通过协同的晶格氧活化与甲基转移调控，实现了高效的甲烷氧化偶联反应活性和催化耐久性。综合表征表明，Sr掺杂ZnO弱化了Sr-O键并增强了电子供体能力，从而有效激活ZnO晶格氧作为甲烷解离的局域氧化剂。同时，金纳米颗粒促进了甲基脱附，抑制了过度氧化并加速了C-C偶联过程。优化后的1%Au/Sr0.05-ZnO催化剂实现了6083.7μmol·g?1·h?1的乙烷产率，选择性高达85.8%。机理研究证实了Sr掺杂介导的Mars-van Krevelen型晶格氧循环机制，其中消耗的晶格氧可通过引入氧气持续补充，确保了催化体系的长期稳定性。该研究为选择性C-H键活化的多功能光催化剂理性设计提供了新的思路。
Abstract	Light-driven oxidative coupling of methane (OCM) to ethane represents a promising strategy for sustainableproduction of value-added chemicals, yet faces challenges due to high activation barriers of C-H bond cleavage. Herein, we demonstrate a dual-site engineered Au/Sr-doped ZnO (Au/Sr-ZnO) photocatalyst that achievesexceptional conversion rates and catalytic durability for OCM through synergistic lattice oxygen activation andmethyl transfer modulation. Comprehensive characterization reveals that Sr doping ZnO weakens Sr-O bondsand enhances electron donation, effectively activating ZnO lattice oxygen as localized oxidants for methanedissociation. Concurrently, Au nanoparticles promote methyl desorption, suppressing over-oxidation while facilitating C-C coupling. The optimized 1%Au/Sr0.05-ZnO catalyst exhibits an ethane production rate of 6083.7 μmol g-1 h-1 with 85.8% selectivity. Mechanistic studies confirm the Mars-van Krevelen-type latticeoxygen cycling mediated by Sr doping, where consumed lattice oxygen is replenished via O2 introduction, ensuring sustained catalytic stability. This work provides new insights into the rational design of multifunctional photocatalysts for selective C-H bond activation.
关键词	光催化；C-H键活化；甲烷氧化偶联；Au/Sr-ZnO；乙烷
KeyWord	Photocatalysis ; C-H activation ; Oxidative coupling of methane; Au/Sr-ZnO; Ethane
基金项目
页码	1-8

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引用本文

王萍, 冯晓燕, 梁军 * , 张金宇, 牛涛涛, 李莉 *. Au/Sr-ZnO双位点工程用于晶格氧活化甲烷高选择性偶联制乙烷 [J]. Applied Catalysis B: Environment and Energy. 2025; 375; (). 1 - 8.

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