Bo Li1, Yuan Si1, Qian Fang1, Ying Shi2, Wei-Qing Huang3, Wangyu Hu4, Anlian Pan1, Xiaoxing Fan5, Gui-Fang Huang6. 1. Department of Applied Physics, College of Physics and Electronics, and College of Materials Science and Engineering, and State Key Laboratory of Chemo/Biosensing and Chemometrics, College of Chemistry and Chemical Engineering, Hunan University, Changsha, 410082, People's Republic of China. 2. Department of Physics and Tsinghua-Foxconn Nanotechnology Research Center, Tsinghua University, Beijing, 100084, People's Republic of China. 3. Department of Applied Physics, College of Physics and Electronics, and College of Materials Science and Engineering, and State Key Laboratory of Chemo/Biosensing and Chemometrics, College of Chemistry and Chemical Engineering, Hunan University, Changsha, 410082, People's Republic of China. wqhuang@hnu.edu.cn. 4. Department of Applied Physics, College of Physics and Electronics, and College of Materials Science and Engineering, and State Key Laboratory of Chemo/Biosensing and Chemometrics, College of Chemistry and Chemical Engineering, Hunan University, Changsha, 410082, People's Republic of China. wyuhu@hnu.edu.cn. 5. College of Physics, Liaoning University, Shenyang, 110036, People's Republic of China. 6. Department of Applied Physics, College of Physics and Electronics, and College of Materials Science and Engineering, and State Key Laboratory of Chemo/Biosensing and Chemometrics, College of Chemistry and Chemical Engineering, Hunan University, Changsha, 410082, People's Republic of China. gfhuang@hnu.edu.cn.
Abstract
Self-assembled nanostructure arrays integrating the advantages of the intrinsic characters of nanostructure as well as the array stability are appealing in advanced materials. However, the precise bottom-up synthesis of nanostructure arrays without templates or substrates is quite challenging because of the general occurrence of homogeneous nucleation and the difficult manipulation of noncovalent interactions. Herein, we first report the precisely manipulated synthesis of well-defined louver-like P-doped carbon nitride nanowire arrays (L-PCN) via a supramolecular self-assembly method by regulating the noncovalent interactions through hydrogen bond. With this strategy, CN nanowires align in the outer frame with the separation and spatial location achieving ultrastability and outstanding photoelectricity properties. Significantly, this self-assembly L-PCN exhibits a superior visible light-driven hydrogen evolution activity of 1872.9 μmol h-1 g-1, rendering a ~ 25.6-fold enhancement compared to bulk CN, and high photostability. Moreover, an apparent quantum efficiency of 6.93% is achieved for hydrogen evolution at 420 ± 15 nm. The experimental results and first-principles calculations demonstrate that the remarkable enhancement of photocatalytic activity of L-PCN can be attributed to the synergetic effect of structural topology and dopant. These findings suggest that we are able to design particular hierarchical nanostructures with desirable performance using hydrogen-bond engineering.
Self-assembled nanostrun class="Chemical">cture arrays integrating the advanpan>tages of the intrinsipan> class="Chemical">c characters of nanostructure as well as the array stability are appealing in advanced materials. However, the precise bottom-up synthesis of nanostructure arrays without templates or substrates is quite challenging because of the general occurrence of homogeneous nucleation and the difficult manipulation of noncovalent interactions. Herein, we first report the precisely manipulated synthesis of well-defined louver-like P-dopedcarbon nitride nanowire arrays (L-PCN) via a supramolecular self-assembly method by regulating the noncovalent interactions through hydrogen bond. With this strategy, CN nanowires align in the outer frame with the separation and spatial location achieving ultrastability and outstanding photoelectricity properties. Significantly, this self-assembly L-PCN exhibits a superior visible light-driven hydrogen evolution activity of 1872.9 μmol h-1 g-1, rendering a ~ 25.6-fold enhancement compared to bulk CN, and high photostability. Moreover, an apparent quantum efficiency of 6.93% is achieved for hydrogen evolution at 420 ± 15 nm. The experimental results and first-principles calculations demonstrate that the remarkable enhancement of photocatalytic activity of L-PCNcan be attributed to the synergetic effect of structural topology and dopant. These findings suggest that we are able to design particular hierarchical nanostructures with desirable performance using hydrogen-bond engineering.