Jin Lu, Cheng Fangyuan, Li Hao, Xie Kui
Key Laboratory of Optoelectronic Materials Chemistry and Physics, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, Fujian, 350002, China.
Key Laboratory of Design & Assembly of Functional Nanostructures, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, Fujian, 350002, China.
Angew Chem Int Ed Engl. 2020 Jun 2;59(23):8891-8895. doi: 10.1002/anie.202001204. Epub 2020 Mar 25.
Porous tantalum nitride (Ta N ) single crystals, combining structural coherence and porous microstructure, would substantially improve the photoelectrochemical performance. The structural coherence would reduce the recombination of charge carriers and maintain excellent transport properties while the porous microstructure would not only reduce photon scattering but also facilitate surface reactions. Here, we grow bulk-porous Ta N single crystals on a two-centimeter scale with (002), (023), and (041) facets, respectively, and show significantly enhanced photoelectrochemical performance. We show the preferential facet growth of porous crystals in a lattice reconstruction strategy in relation to lattice match and lattice channel. We present the facet engineering to enhance light absorption, exciton lifetime and transport properties. The porous Ta N single crystal boosts photoelectrochemical oxidation of alcohols with the (002) facet showing the highest performance of >99 % alcohol conversion and >99 % aldehyde/ketone selectivity.
多孔氮化钽（TaN）单晶兼具结构连贯性和多孔微结构，将大幅提升光电化学性能。结构连贯性可减少电荷载流子的复合并维持优异的传输特性，而多孔微结构不仅能减少光子散射，还能促进表面反应。在此，我们分别在两厘米尺度上生长出具有（002）、（023）和（041）晶面的块状多孔TaN单晶，并展现出显著增强的光电化学性能。我们展示了在晶格重构策略中，多孔晶体相对于晶格匹配和晶格通道的优先晶面生长。我们提出了晶面工程以增强光吸收、激子寿命和传输特性。多孔TaN单晶促进了醇类的光电化学氧化，其中（002）晶面表现出最高性能，醇转化率>99%，醛/酮选择性>99%。
