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Ag2CrO4/g-C3N4/graphene oxide ternary nanocomposite Z-scheme photocatalyst with enhanced CO2 reduction activity
Applied Catalysis B: Environment and Energy ( IF 20.2 ) Pub Date : 2018-03-11 , DOI: 10.1016/j.apcatb.2018.03.036
Difa Xu , Bei Cheng , Weikang Wang , Chuanjia Jiang , Jiaguo Yu

Graphitic carbon nitride (g-C3N4)-based photocatalysts holds great promise on photocatalytic CO2 conversion into solar fules; however, the efficiency of pristine g-C3N4 is currently limited by its poor visible light absorption and rapid charge recombination. Employing silver chromate (Ag2CrO4) nanoparticles as photosensitizer and graphene oxide (GO) as cocatalyst, a novel ternary Ag2CrO4/g-C3N4/GO composite photocatalyst was fabricated for photocatalytic CO2 reduction into methanol (CH3OH) and methane (CH4). The ternary composites exhibited an enhanced CO2 conversion activity with a turnover frequency of 0.30 h–1, which was 2.3 times that of pristine g-C3N4 under simulated sunlight irradiation. The enhanced photocatalytic activity was due to broadened light absorption, higher CO2 adsorption and more efficient charge separation. Specifically, due to the matched band structure and appropriate loading ratio of Ag2CrO4, a direct Z-scheme Ag2CrO4/g-C3N4 heterojunction is formed, driven by the internal electric field across the Ag2CrO4/g-C3N4 interface. The formation of the direct Z-scheme heterojunction is substantiated by radical scavenging experiments and density functional theory calculations, and it benefits the photocatalytic reaction by accelerating the charge separation and improving the redox ability. Furthermore, GO cocatalyst not only promotes the charge transfer but also provides plentiful CO2 adsorption and catalytic sites. This work exemplifies the facile development of ternary g-C3N4-based photocatalysts with high CO2-conversion activity by coupling a small amount of Ag-based photosensitizer and metal-free cocatalyst.



中文翻译:

具有增强的CO 2还原活性的Ag 2 CrO 4 / gC 3 N 4 /氧化石墨烯三元纳米复合Z方案光催化剂

石墨化的氮化碳(gC 3 N 4)基光催化剂在将光催化的CO 2转化为太阳能电池方面具有广阔的前景。然而,原始的gC 3 N 4的效率目前受到可见光吸收差和电荷快速重组的限制。以铬酸银(Ag 2 CrO 4)为光敏剂,氧化石墨烯(GO)为助催化剂,制备了新型三元Ag 2 CrO 4 / gC 3 N 4 / GO复合光催化剂,用于将CO 2光催化还原为甲醇(CH 3)。OH)和甲烷(CH 4)。在模拟阳光照射下,三元复合材料显示出增强的CO 2转化活性,转换频率为0.30 h –1,是原始gC 3 N 4的2.3倍。增强的光催化活性归因于更宽的光吸收,更高的CO 2吸附和更有效的电荷分离。具体地,由于匹配的能带结构和Ag 2 CrO 4的合适的负载比,直接Z方案Ag 2 CrO 4 / gC 3 N 4在内部电场的作用下,跨Ag 2 CrO 4 / gC 3 N 4界面形成异质结。直接Z方案异质结的形成通过自由基清除实验和密度泛函理论计算得到证实,并且它通过加速电荷分离和提高氧化还原能力而有益于光催化反应。此外,GO助催化剂不仅促进电荷转移,而且提供大量的CO 2吸附和催化位点。这项工作例证了具有高CO 2的三元基于gC 3 N 4的三元光催化剂的简便开发偶合少量的基于银的光敏剂和不含金属的助催化剂可实现高转化活性。

更新日期:2018-03-11
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