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协同原子共掺杂与S型异质结:利用罗勒籽衍生的超薄类石墨烯碳构建Cu/CuO/CuO用于增强苯甲醇光氧化制醛

Synergistic atom co-sharing and S-scheme heterojunction: constructing Cu/CuO/CuO with ultrathin graphene-like carbon derived from basil seeds for enhanced photo-oxidation of benzyl alcohols to aldehydes.

作者信息

Nalkyashree Zahra Kohansal, Koukabi Nadiya, Dashtian Kheibar, Seidi Farzad

机构信息

Department of Chemistry, Semnan University P.O. Box 35131-19111 Semnan Iran

Department of Chemistry, Iran University of Science and Technology Tehran 16846-13114 Iran

出版信息

Nanoscale Adv. 2024 Sep 2;6(21):5348-60. doi: 10.1039/d4na00283k.

Abstract

This study is centered on the oxidative transformation of alcohols into their respective aldehyde compounds, employing an S-scheme heterostructure featuring CuO/CuO on graphene-like carbon (GLC) derived from a basil seed hydrogel. Experimental characterization and theoretical calculations highlight that the implementation of S-scheme heterostructures achieves not only enhanced charge-separation efficiency, facilitated by the interfacial built-in electric field, Cu co-sharing at the CuO/CuO interface, and electron carrier activity of the GLC support, but also maintains a strong driving force for photocatalytic organic conversion. The resulting nanocomposites play a crucial role in transferring and reducing the recombination of photoexcited charge carriers, preserving the oxidizability of CuO holes and the reducibility of CuO electrons. Through meticulous adjustment of precursor amounts, the CuO-CuO/GLC heterojunction exhibited the highest photocurrent at 6.83 mA cm, demonstrating optimal performance in the photocatalytic selective oxidation of benzyl alcohol with an average conversion rate of 95.0%. Furthermore, the stability of CuO-CuO/GLC was thoroughly investigated, revealing sustained high conversion even after five repeated experiments, underscoring its potential for practical applications. The study also proposes a plausible mechanism for the transformation of benzyl alcohol into benzaldehyde through capture experiments of active species. Importantly, this research introduces a straightforward hydrothermal growth protocol for efficiently constructing metal oxide heterostructures wrapped in an rGO support. It provides valuable insights into designing new synthetic strategies for preparing efficient photocatalysts and hints at the development of novel, efficient, and practical photocatalytic systems.

摘要

本研究聚焦于醇类向其相应醛类化合物的氧化转化,采用了一种S型异质结构,该结构以来源于罗勒籽水凝胶的类石墨烯碳(GLC)上的CuO/CuO为特征。实验表征和理论计算表明,S型异质结构的实施不仅实现了电荷分离效率的提高,这得益于界面内建电场、CuO/CuO界面处的Cu共享以及GLC载体的电子载体活性,而且还保持了光催化有机转化的强大驱动力。所得的纳米复合材料在转移和减少光激发电荷载流子的复合方面发挥着关键作用,保持了CuO空穴的氧化性和CuO电子的还原性。通过对前驱体用量的精心调整,CuO-CuO/GLC异质结在6.83 mA cm时表现出最高的光电流,在苯甲醇的光催化选择性氧化中展现出最佳性能,平均转化率为95.0%。此外,还对CuO-CuO/GLC的稳定性进行了深入研究,结果表明即使经过五次重复实验仍能保持高转化率,突出了其实际应用潜力。该研究还通过活性物种捕获实验提出了苯甲醇转化为苯甲醛的合理机制。重要的是,本研究引入了一种简单的水热生长方案,用于高效构建包裹在rGO载体中的金属氧化物异质结构。它为设计制备高效光催化剂的新合成策略提供了有价值的见解,并为新型、高效和实用的光催化系统的开发提供了线索。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/dfdf/11495273/cfa19024c6c8/d4na00283k-f2.jpg

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