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Biomimetic inspired porphyrin-based nanoframes for highly efficient photocatalytic CO2 reduction
Chemical Engineering Journal ( IF 13.3 ) Pub Date : 2021-01-07 , DOI: 10.1016/j.cej.2021.128414
Shujie Liang , Xiaohui Zhong , Zuqi Zhong , Bin Han , Weiyi Chen , Kainan Song , Hong Deng , Zhang Lin

The development of biomimetic catalysis for efficient photoreduction of CO2 is an effective alternative to address energy problems. However, amelioration on the construction of biomimetic catalysts for elevated photocatalytic performance is still challenging and demanded. Herein, a bioinspired artificial photosynthesis system is constructed based on ZrO2 nanoframes (ZFs) and metalloporphyrin to mimic the morphology of trees. The robust backbone of the framework and the bio-inspiring porphyrins anchored on the surface of ZFs function as the strong trunk and well-ordered leaves of a tree, respectively. The biomimetic system achieves an evolution yield of 35.3 μmol during 3 h reaction with 93.1% CO selectivity and 1.84% CO apparent quantum efficiency (A.Q.E.), which is about 60.8 times larger than that of pure porphyrin (Ni) (0.58 μmol). Detailed analysis reveals that the catalytic system could not only achieve fast separation of the photogenerated carriers and effective CO2 activation but also possess suitable energy levels, which could efficiently transfer electrons to the Ni catalytic sites to improve the photocatalytic activity. Furthermore, the good recycling tests could be explained by the robust supporting of frameworks as well as the strong binding of the Zr atoms and carboxyl groups of porphyrins. This work presents a simple model of biomimetic catalysts and outlines possible strategies for other biomimetic manufactures.



中文翻译:

仿生启发性的基于卟啉的纳米框架,可实现高效的光催化CO 2还原

用于有效光还原CO 2的仿生催化的发展是解决能源问题的有效替代方法。然而,改善仿生催化剂的结构以提高光催化性能仍然是具有挑战性和要求的。本文中,基于ZrO 2纳米框架(ZFs)和金属卟啉构建了仿生的人工光合作用系统,以模仿树木的形态。框架的坚固骨架和锚定在ZF表面上的具有生物启发性的卟啉分别起着树的强壮树干和井井有条的作用。仿生系统在3 h反应中达到35.3μmol的析出产率,具有93.1%的CO选择性和1.84%的CO表观量子效率(AQE),约为纯卟啉(Ni)(0.58μmol)的60.8倍。详细分析表明,该催化体系不仅可以实现光生载流子的快速分离和有效的CO 2活化,而且具有合适的能级,可以有效地将电子转移到Ni催化位上,从而提高了光催化活性。此外,良好的回收利用测试可以通过强大的骨架支撑以及卟啉的Zr原子和羧基的牢固结合来解释。这项工作提出了一个仿生催化剂的简单模型,并概述了其他仿生产品的可能策略。

更新日期:2021-01-18
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