Tuning the N-bonded cerium(iii) fraction/g-C3N4 interface in hollow structures using an: In situ reduction treatment for superior photochemical hydrogen evolution

Waqas，Muhammad1; Yang，Bo1; Cao，Lujie3; Zhao，Xu2; Iqbal，Waheed1; Xiao，Ke1; Zhu，Caizhen1; Zhang，Junmin1

2019

10.1039/c9cy01305a

Catalysis Science & Technology   影响因子和分区

2044-4753

2044-4761

The synthesis of inorganic/organic interfaces in spherical hollow structures (HS) is a promising but challenging task. Herein, we innovatively utilized porous CeO-HS as a scaffold to incorporate cyanamide molecules, which upon one-step in situ reducing treatment, yielded nitrogen-bonded CeO/g-CN-HS. The electron microscope and spectroscopic analysis validated two functions of cyanamide: I) it generates an in situ reducing atmosphere (CO, N, NO) to tune the cerium oxide vacancy population, and ii) it acts as a N and g-CN precursor. Meanwhile, the unique HS geometry promotes cerium oxide reduction at low temperature due to the following: I) the high surface area of CeO-HS provides a larger area for CeO/CO interaction; ii) adequate pore volume enhances the cerium oxide reduction kinetics; and, iii) the CeO nanoparticles increase the ceria surface defect population by obeying the ceria oxygen vacancy transport model. Remarkably, the N-CeO/g-CN-HS photocatalyst hydrogen evolution rate is 43.32 μmol g h under visible light (λ ≥ 420 nm), which is 3.8 times higher than pristine g-CN (11.4 μmol g h) due to: A) enhancement of the material's light-harvesting ability by HS, b) formation of controlled optically active Ce sites, and c) intimate inorganic/organic interfaces, which boosted the minority carriers' separation efficiency.

SCI ; EI

英语

其他

National Major Science & Technology Program for Water Pollution Control Treatment[2017ZX07202]

Chemistry

Chemistry, Physical

WOS:000496289200007

ROYAL SOC CHEMISTRY

20194307573633

Hydraulic structures ; Hydrogen ; Light ; Oxides ; Reduction ; Scaffolds ; Spectroscopic analysis ; Surface defects ; Temperature

Construction Equipment:405.1 ; Thermodynamics:641.1 ; Light/Optics:741.1 ; Chemistry:801 ; Chemical Reactions:802.2 ; Chemical Products Generally:804 ; Materials Science:951

2-s2.0-85073679660

Scopus

1.College of Chemistry and Environmental EngineeringShenzhen University,Shenzhen,518060,China
2.Key Laboratory of Drinking Water Science and TechnologyResearch Center for Eco-Environmental SciencesChinese Academy of Sciences,Beijing,100085,China
3.Department of Material Science and EngineeringSouthern University of Science and Technology,Shenzhen,518055,China

Waqas，Muhammad,Yang，Bo,Cao，Lujie,et al. Tuning the N-bonded cerium(iii) fraction/g-C3N4 interface in hollow structures using an: In situ reduction treatment for superior photochemical hydrogen evolution[J]. Catalysis Science & Technology,2019,9(19):5322-5332.

Waqas，Muhammad.,Yang，Bo.,Cao，Lujie.,Zhao，Xu.,Iqbal，Waheed.,...&Zhang，Junmin.(2019).Tuning the N-bonded cerium(iii) fraction/g-C3N4 interface in hollow structures using an: In situ reduction treatment for superior photochemical hydrogen evolution.Catalysis Science & Technology,9(19),5322-5332.

Waqas，Muhammad,et al."Tuning the N-bonded cerium(iii) fraction/g-C3N4 interface in hollow structures using an: In situ reduction treatment for superior photochemical hydrogen evolution".Catalysis Science & Technology 9.19(2019):5322-5332.