期刊
ACS APPLIED MATERIALS & INTERFACES
卷 11, 期 28, 页码 25186-25194出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsami.9b06264
关键词
artificial photosynthesis; photocatalyst; CO2 reduction; black TiO2; interfacial dipole; solar fuel
资金
- Ministry of Science and Technology (MOST) in Taiwan [105-2745-M-002-003-ASP, 106-2745-M-002-002-ASP, 107-2745-M-002-001-ASP]
- Deep Decarbonization Project under Academia Sinica [AS-SS-106-02-3]
- Center of Atomic Initiative for New Materials (AI-Mat), National Taiwan University from the Featured Areas Research Center Program by the Ministry of Education (MOE) in Taiwan [107L9008]
Tuning the electronic band structure of black titania to improve photocatalytic performance through conventional band engineering methods has been challenging because of the defect-induced charge carrier and trapping sites. In this study, KSCN-modified hydrogenated nickel nano cluster-modified black TiO2 (SCN-H-Ni-TiO2) exhibits enhanced photocatalytic CO2 reduction due to the interfacial dipole effect. Upon combining the experimental and theoretical simulation approach, the presence of an electrostatic interfacial dipole associated with chemisorption of SCN has dramatic effects on the photocatalyst band structure in SCN H-Ni-TiO2. An interfacial dipole possesses a more negative zeta potential shift of the isoelectric point from 5.20 to 3.20, which will accelerate the charge carrier separation and electron transfer process. Thiocyanate ion passivation on black TiO2 demonstrated an increased work function around 0.60 eV, which was induced by the interracial dipole effect. Overall, the SCN H-Ni-TiO2 photocatalyst showed an enhanced CO2 reduction to solar fuel yield by 2.80 times higher than H-Ni-TiO2 and retained around 88% product formation yield after 40 h.
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