Merging Single-Atom-Dispersed Iron and Graphitic Carbon Nitride to a Joint Electronic System for High-Efficiency Photocatalytic Hydrogen Evolution

Zhang, Wenyao1,2; Peng, Qiong1; Shi, Lingling1; Yao, Qiushi3; Wang, Xin1; Yu, Aiping2; Chen, Zhongwei2; Fu, Yongsheng1

2019-11-14

10.1002/smll.201905166

Small   影响因子和分区

1613-6810

1613-6829

Scalable and sustainable solar hydrogen production via photocatalytic water splitting requires extremely active and stable light-harvesting semiconductors to fulfill the stringent requirements of suitable energy band position and rapid interfacial charge transfer process. Motivated by this point, increasing attention has been given to the development of photocatalysts comprising intimately interfaced photoabsorbers and cocatalysts. Herein, a simple one-step approach is reported to fabricate a high-efficiency photocatalytic system, in which single-site dispersed iron atoms are rationally integrated on the intrinsic structure of the porous crimped graphitic carbon nitride (g-C3N4) polymer. A detailed analysis of the formation process shows that a stable complex is generated by spontaneously coordinating dicyandiamidine nitrate with iron ions in isopropanol, thus leading to a relatively complicated polycondensation reaction upon thermal treatment. The correlation of experimental and computational results confirms that optimized electronic structures of Fe@g-C3N4 with an appropriate d-band position and negatively shifting Fermi level can be achieved, which effectively gains the reducibility of electrons and creates more active sites for the photocatalytic reactions. As a result, the Fe@g-C3N4 exhibits a highlighted intramolecular synergistic effect, performing greatly enhanced solar-photon-driven activities, including excellent photocatalytic hydrogen evolution rate (3390 mu mol h(-1) g(-1), lambda > 420 nm) and a reliable apparent quantum efficiency value of 6.89% at 420 nm.

d-band position graphitic carbon nitride photocatalytic hydrogen evolution single-atom catalysis synergistic active centers

SCI ; EI

英语

其他

Fundamental Research Funds for the Central Universities[30917015102] ; Fundamental Research Funds for the Central Universities[30918014103]

Chemistry ; Science & Technology - Other Topics ; Materials Science ; Physics

Chemistry, Multidisciplinary ; Chemistry, Physical ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary ; Physics, Applied ; Physics, Condensed Matter

WOS:000496318800001

WILEY-V C H VERLAG GMBH

20194707719211

Atoms ; Carbon nitride ; Charge transfer ; Electronic structure ; Hydrogen production ; Metal ions ; Nitrides ; Photocatalytic activity ; Solar power generation

Gas Fuels:522 ; Metallurgy:531.1 ; Solar Power:615.2 ; Chemical Reactions:802.2 ; Inorganic Compounds:804.2 ; Atomic and Molecular Physics:931.3

Web of Science

1.Nanjing Univ Sci & Technol, Key Lab Soft Chem & Funct Mat, Minist Educ, Nanjing 210094, Jiangsu, Peoples R China
2.Univ Waterloo, Waterloo Inst Nanotechnol, Waterloo, ON N2L 3G1, Canada
3.Southern Univ Sci & Technol, Dept Phys, Shenzhen 518055, Peoples R China

Zhang, Wenyao,Peng, Qiong,Shi, Lingling,et al. Merging Single-Atom-Dispersed Iron and Graphitic Carbon Nitride to a Joint Electronic System for High-Efficiency Photocatalytic Hydrogen Evolution[J]. Small,2019,15(50).

Zhang, Wenyao.,Peng, Qiong.,Shi, Lingling.,Yao, Qiushi.,Wang, Xin.,...&Fu, Yongsheng.(2019).Merging Single-Atom-Dispersed Iron and Graphitic Carbon Nitride to a Joint Electronic System for High-Efficiency Photocatalytic Hydrogen Evolution.Small,15(50).

Zhang, Wenyao,et al."Merging Single-Atom-Dispersed Iron and Graphitic Carbon Nitride to a Joint Electronic System for High-Efficiency Photocatalytic Hydrogen Evolution".Small 15.50(2019).