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Carbon dots-triggered the fabrication of miniature g-C3N4/CDs/WO3 S-scheme heterojunction for efficient CO2 photoreduction
Chemical Engineering Journal ( IF 13.3 ) Pub Date : 2023-10-18 , DOI: 10.1016/j.cej.2023.146774
Xiangguang Kong , Jiajie Fan , Bingwei Feng , Jun Li , Guidong Yang , Chao Xue

Production of high value-added solar fuels from sunlight and carbon dioxide (CO2) have attracted much interest for achieving carbon neutrality, yet the current photocatalytic CO2 reduction reaction (CRR) process still suffers from inactivation of inert molecules and severe charge recombination. Here, we report a versatile carbon dots (CDs)-triggered confined co-assembly strategy to integrate ultrafine tungsten trioxide (WO3)/CDs quantum dots with graphitic carbon nitride (g-C3N4) for the fabrication of miniature g-C3N4/CDs/WO3 Step-scheme (S-scheme) heterojunction. Without any sacrificial reagent, the optimal photocatalyst enables 99.5 % selectivity toward the production of CO, with the highest yield rate of 31.04 µmol‧g−1‧h−1 under the gas–solid phase reaction. In situ spectra investigation and density functional theory (DFT) calculations suggest that the bifunctional CDs not only trigger quantum-sized precise assembly of WO3 nanocrystal on the surface of g-C3N4 matrix without aggregation, but also mediate the interfacial charge transportation. Moreover, the established S-scheme electron transfer pathway favor the rapid charge separation and directional transfer, thus ensuring the maximum utilization of photo-generated charge carriers for efficient photocatalytic CRR. This work provides a new tactic for rational design and synthesis CDs-mediated S-scheme heterojunction to harness solar energy into high value-added solar fuel.



中文翻译:

碳点触发微型 g-C3N4/CDs/WO3 S 型异质结的制造,用于有效的 CO2 光还原

利用阳光和二氧化碳(CO 2 )生产高附加值太阳能燃料对于实现碳中和引起了人们的广泛关注,但目前的光催化CO 2还原反应(CRR)过程仍然存在惰性分子失活和严重的电荷重组的问题。在这里,我们报告了一种多功能碳点(CD)触发的限域共组装策略,将超细三氧化钨(WO 3)/CDs量子点与石墨氮化碳(gC 3 N 4)集成,用于制造微型gC 3 N 4 /CDs/WO 3阶梯式(S 式)异质结。在没有任何牺牲试剂的情况下,最佳光催化剂对CO的产生具有99.5%的选择性,在气固相反应下最高产率为31.04 µmol‧g -1 ‧h -1 。原位光谱研究和密度泛函理论(DFT)计算表明,双功能CD不仅可以在gC 3 N 4基质表面触发量子尺寸的WO 3纳米晶体的精确组装而不聚集,而且还可以介导界面电荷传输。此外,所建立的S型电子转移路径有利于电荷的快速分离和定向转移,从而确保最大限度地利用光生电荷载流子,实现高效的光催化CRR。这项工作为合理设计和合成CDs介导的S型异质结以将太阳能转化为高附加值太阳能燃料提供了一种新策略。

更新日期:2023-10-18
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