Baofang Zhang,Ziyu Zengcai,Wenting Lin,Meijin Zhang,Yunhong Pi,Tiejun Wang
Photothermal synergism can effectively activate methanol at low operating temperature and significantly reduce the activation energy of the reaction, achieving more efficiently H 2 release from methanol reforming. Here, a novel hierarchical heterojunction that integrating photo- and thermal-active Cu 2 O catalytic species with in-situ derived NH 2 -MIL-125@TiO 2 framework was specifically designed for photothermal-driven aqueous phase reforming of methanol into H 2 . The afforded Cu 2 O/NH 2 -MIL-125@TiO 2 realized an outstanding photothermal H 2 production activity (apparent quantum efficiency of 22.3 % at 365 nm), ca. 13-times higher than that of thermocatalytic condition. Interestingly, the photothermal effect did confer the Cu 2 O/NH 2 -MIL-125@TiO 2 with unexpected activity at low temperature subsided to 100 °C and accelerated the activation of MeOH/H 2 O with an obvious reduction of activation energy from 82.62 kJ·mol −1 to 52.40 kJ·mol −1 . The improvement of catalyst stability and the promotion of charge separation also contributed to a long-term photothermal H 2 evolution activity with average rate of 1.49x10 6 μmolg Cu -1 h −1 and a total turnover number (TON) up to 5971 in 63 h, almost 125-fold promotion compared with Cu 2 O.
Weicheng Cui,Jianpeng Shang,Hongye Bai,Jian Hu,Dongbo Xu,Jinrui Ding,Weiqiang Fan,Weidong Shi
Realizing a highly efficient catalytic activity for photoelectrochemical (PEC) water splitting has been becoming a key challenge for fabricating TiO 2 photoanode, due to its weak light-response ability and poor electrical conductivity. For the first time, we prepared the TiO 2 nanorods decorated with NH 2 -MIL-125 film, and subsequently in-situ implanted Ag nanoparticles (Ag NPs) into NH 2 -MIL-125 film by mild reduction process with the help of amine group. The synergistic effect between NH 2 -MIL-125 and Ag NPs is aimed at efficiently improving light-response and the overall conductivity of photoanode. The PEC performance of as-prepared Ag/NH 2 -MIL-125/TiO 2 hybrid-photoanode has been systemically investigated. The photocurrent density of optimal Ag/NH 2 -MIL-125/TiO 2 has reached 1.06 mA/cm 2 at 1.23 V (vs. RHE) under illumination (100 mW/cm 2 ), which is almost 4.42 times higher than that of pristine TiO 2 . The incident photon-to-electron conversion efficiency (IPCE) value of Ag/NH 2 -MIL-125/TiO 2 has been increased to 51.0% at 390 nm. Furthermore, the desirable charge injection ( η i n j e c t i o n ) of 96.4% and charge separation ( η s e p a r a t i o n ) efficiency of 33.1% have been achieved. The in-situ introduction of Ag NPs into NH 2 -MIL-125/TiO 2 heterostructure provides a novel model for understanding the synergistic effect between metal and MOF over PEC water splitting.
Yang Wen,Wang Yujia,Gao Na,Zhu Zhengfa,Chen Yuanyuan,Wang Hao,Tang Xiaoning
Designing efficient visible light-driven photocatalytic antimicrobial agents presents significant challenges. In this study, S-shaped core–shell NH 2 -MIL-125/TiO 2 (NT-x) heterojunctions were constructed by simple in situ solvothermal method, as photocatalytic antimicrobial agents for efficient bactericidal use under visible light. Notably, 99.99% inhibition was achieved for both Escherichia coli and Staphylococcus aureus at low concentrations (0.02 and 0.035 mg mL −1 , respectively) after exposure to simulated sunlight for 20 min. Reasonable energy band configuration and built-in electric field of this structure provided improved photogenerated carrier transfer paths as well as enhanced separation and transport efficiency. Moreover, the core–shell structure enhanced the interaction between NH 2 -MIL-125 and TiO 2 , increased the total number of reactive sites, and promoted the efficient generation of reactive oxygen species. Finally, possible mechanisms for the inactivation of bacteria were discussed. This research offers new perspectives for the advancement of advanced metal–organic framework-based photocatalysts with antibacterial activity under visible light. Graphical abstract
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