JOURNAL OF MEMBRANE SCIENCE
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2026
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IF 9
Xiaochan An,Yutong Gu,Wenping Wang,Jianxiao Wang,Yongxin Cui,Hongbing Luo,Ke Zhang,Liangqian Fan,Wei Chen
Membrane-fouling in forward osmosis (FO) process has limited its application in drug-containing wastewater treatment. Advanced membrane coupled photocatalytic oxidation process has drawn growing interest. In this study, functional photocatalytic thin-film composite (TFC) membranes modified using metal-organic framework of NH 2 -MIL-125(Ti) (NM125) were prepared through simple blending during interfacial polymerization process. Due to the intrinsic hydrophilicity and photocatalytic properties of the nano-sized NM125, the modified TFC membrane (NM-6) demonstrates improved permeability-selectivity with a A/B value of 16.19 bar -1 , outstanding light-response functionality (the photocatalytic efficiency is 80.95 % for tetracycline hydrochloride (THC) and 66.76 % for ibuprofen (IBU)), and ∼100 % rejection of THC and IBU in nearly all the FO tests. Furthermore, NM-6 displays excellent operation stability with a 5 % water decline and 98 % water recovery for treating THC-containing feed solution under light irradiation (0.64 kW/m 2 ), while the control membrane of NM-0 showed 22 % of water decline and 85 % water recovery. Our membrane with the property of photocatalytic self-cleaning opens opportunities for developing next-generation anti-fouling forward osmosis membranes.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2026
·
IF 19.7
Wanyin Xu,Yuanhao Chen,Tianhe Gao,Zihan Wang,Wenkang Miao,Peng Wang,Qianqian Li
Successfully tailored a dual-site architecture comprising Cu + /Ni δ+ -O V -Ti and CuNi NPs on the ultra-small TiO 2 support-derived from MIL-125(Ti). • Deeply revealed the defect rich Cu + /Ni δ+ -O V -Ti site promotes CO 2 adsorption, while the CuNi NPs with electron redistribution facilitates H 2 adsorption and desorption of the product CO. • Significantly enhanced the RWGS reaction activity and sintering-resistance. Copper (Cu)-based catalysts hold promise for the reverse water-gas shift (RWGS) reaction because of their 100% selectivity toward CO. However, their low intrinsic activity, and deactivation caused by irreversible sintering during RWGS reaction remain persistent challenges. Herein, we report a pore adsorption strategy to simultaneously achieve electronic structure modulation and preserve microstructure stability during the RWGS reaction. Specifically, a MOF-derived TiO 2 -supported CuNi catalyst is constructed with dual active sites consisting of Cu + /Ni δ+ -O V -Ti sites and CuNi nanoparticles (NPs). The optimized catalytic performance achieves CO 2 conversion of 37.1% with CO selectivity of 99.9% and operates stably for 200 h at 450 ℃, placing its performance among the advanced Cu-based catalysts reported to date. Atomic/electronic structure characterization and density functional theory calculations demonstrate that Cu + /Ni δ+ -O V -Ti sites with enhanced charge redistribution capability promote CO 2 adsorption. The CuNi NP sites with electronic interaction enhance H 2 adsorption and moderate CO adsorption. This work provides a rational design strategy for highly active, selective and stable Cu-based RWGS catalysts. Download: Download high-res image (286KB) Download: Download full-size image Dual active sites consisting of Cu + /Ni δ+ -O V -Ti sites and CuNi NPs are constructed in the MOF-derived CuNi/TiO 2 catalyst, enabling electronic modulation and structural stabilization for enhanced RWGS reaction.
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DALTON TRANSACTIONS
·
2023
·Vol. 52
·期 11
·3517-3525
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IF 4
Shihui Wang,Zhoujun He,Ling Wu,Deling Wang,Ruiru Si,Xiyao Liu,Ruowen Liang
Due to their explicit structure, metal–organic frameworks (MOFs) have been supposed to be credible platforms to research the micro-mechanism of heterogeneous photocatalysis. In this study, amino-functionalized MOFs (MIL-125(Ti)–NH2 (denoted as MTi), UiO-66(Zr)–NH2 (denoted as UZr) and MIL-68(In)–NH2 (denoted as MIn)) with three different metal centers were synthesized and applied for the denitrification of simulated fuels under visible light irradiation, during which pyridine was used as a typical nitrogen-containing compound. The results showed that MTi had the best activity among the above three MOFs, and the denitrogenation rate increased to 80% after 4 h of visible light irradiation. On the grounds of the theoretical calculation of pyridine adsorption and actual activity experiments, it can be presumed that the unsaturated Ti4+ metal centers should be the key active sites. Meanwhile, the XPS and in situ infrared results verified that the coordinatively unsaturated Ti4+ sites facilitate the activation of pyridine molecules through the surface –N⋯Ti– coordination species. The coordination–photocatalysis synergism promotes the efficiency of photocatalytic performance and the corresponding mechanism is proposed.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2022
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IF 6.371
Zhicheng Zhang,Chao Xu,Xudong Xiong,Chen Wang,Qi Zhang,Zhao Fan,Yongqian Wang
The application of CdS in pollutant degradation was limited due to the rapid compounding of photogenerated carriers. A ternary Au@NH 2 -MIL-125(Ti)/CdS (5Au@40NMT/CdS) composite catalyst was synthesized with a two-step method and methylene blue (MB) was used as simulate contaminants to evaluate its photocatalytic performance under simulated visible light. The compounding of NH 2 -MIL-125 and the loading of Au nanoparticles significantly enhanced the photodegradation performance of the composite catalyst. Compared with pure CdS, the ternary composite catalyst exhibited higher degradation efficiency (93.3 %) and higher degradation rate (9 times that of CdS)within 30 min, which was attributed to the high specific surface area and the synergistic effect of the three components that accelerated the carrier separation and broadened the photoresponse range. In addition, superoxide radical (·O 2 - ) was identified as the main active species in the MB degradation process by the electron spin resonance (ESR) technique. This work was expected to give a strategy for the fabrication and design of CdS/MOF composite catalysts in the field of pollutant degradation.
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CHEMOSPHERE
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2022
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IF 8.943
Hongyu Lu,Chengxun Deng,Zhimin Yu,Dianya Zhang,Weiping Li,Jun Huang,Teng Bao,Xiaowei Liu
Plasma techniques to degrade pollutants are generally more efficient than conventional methods, but exist some problems such as high energy consumption, incomplete degradation of pollutants, and secondary pollution caused by highly toxic intermediates. In this study, the dielectric barrier discharge plasma (DBDP) combined with the Ti-based metal organic frameworks (MOFs) catalysts (P25/NH 2 -MIL-125(Ti)) was used to degrade fluorene in the soil. The synergistic treatment technique used in soil remediation can realize a green and promising treatment efficiency with relatively low energy consumption. Compared with DBDP system alone, the synergetic treatment system of DBDP and P25/NH 2 -MIL-125(Ti) considerably increased the degradation efficiency of fluorene in the soil to above 90% at 10 min, even with a relatively low discharge voltage (5 kV). The synergistic treatment system achieved 88.8% of fluorene mineralization at 60 min. Optical emission spectroscopy and electron paramagnetic resonance spectroscopy both showed that •OH and •O 2 − played an important role in the synergetic treatment system. Nine main intermediates were identified using gas chromatography-mass spectrometry and Fourier transform infrared analysis. The main degradation of fluorine in soil was caused by the electronic transition of the catalytic material excited by DBDP, and finally mineralized into CO 2 and H 2 O. The fluorene and its toxic intermediates were effectively removed. This study provides an insight for achieving high efficiency and environmentally friendly application perspective in soil remediation.
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OPTICAL MATERIALS
·
2021
·
IF 3.08
Yang Wang,Sheng Feng,Wei Wu,Yun Zhou,Zhiwei Ye,Xiaojun Dai,Xun Cao
In this article, we reported a method for synthesizing cluster-like NH 2 -MIL-125(Ti)/BiOBr (NMT/B) Z type heterojunction composite materials with different content by using ionic liquid as bromine source assisted solvothermal method. In visible light , the photocatalytic activity of the materials was analyzed by degradation of tetracycline. Characterize the prepared composite material by XRD , FTIR, SEM, TEM, XPS , UV–vis diffuse reflection spectra (DRS). The result proved that the NH2-MIL-125(Ti) (NMT) nanosheets were tightly loaded on the BiOBr surface. NMT/B composite materials showed higher catalytic activity than monomer materials. The removal rate of TC reached 88% in 90min, which was 3 times and 5.7 times that of the monomer NMT and BiOBr monomer materials, respectively. In the catalytic process, –O 2 - and h + are the main active substances that degrade pollutants. This is proved by free radical capture experiments. It could be inferred that the improved photocatalytic activity of NMT/B composites was contributed to the good energy band structure and the formation of Z-type heterojunctions in close contact, which greatly facilitates the photogenerated carrier and hole migration and dissociation. Cycle experiment proved that the prepared composite material has excellent stability, which indicated that it had a good prospect in practical applications.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2020
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IF 3.573
Meijuan Chen,Xiaoyan Wei,Liaoliao Zhao,Yu Huang,Shun-cheng Lee,Wingkei Ho,Kehao Chen
Highly efficient and stable photocatalysts were synthesized at room temperature by modifying MIL-125(Ti) with N-doped carbon quantum dots (N/CM(Ti)). The N/CM(Ti) with 2.5 vol % N doped carbon quantum dots (N/CQDs) had the best light absorption and visible-light photocatalytic nitrogen oxide (NO) removal efficiency (approximately 49%). It was found through X-ray photoelectron spectroscopy analysis that a N–Ti–O bond was formed in the 2.5 vol % N/CM(Ti), which is more conducive to charge transfer. Photocurrent and electrochemical impedance data also showed that the carrier separation efficiency of 2.5 vol % N/CM(Ti) was significantly superior to that of MIL-125(Ti). In addition, the TiIII–TiIV of MIL-125(Ti) acts as the active center for photocatalytic removal of NO. Two possible electron migration paths were proposed: electron transfer from N/CQDs to TiIII–TiIV center of MIL-125(Ti) due to the photoinduced electron transfer property of N/CQDs, and absorption of UV light generated from the N/CQDs by the terephthalic acid ligand followed by electron transfer to metal active sites for photocatalytic removal of NO.
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RSC Advances
·
2019
·Vol. 9
·期 57
·33238-33245
·
IF 3.049
Zhi Li,Guangbo Che,Wei Jiang,Lihui Liu,Hairui Wang
In the present study, a novel photocatalyst, CQDs@MIL-125(Ti) (CQDs = carbon quantum dots), was prepared via a solvothermal procedure. The photocatalytic properties were tested by the degradation of tetracycline (TC) with a 250 W Xe lamp (λ > 420 nm). Compared with pure MIL-125(Ti), the 10 wt% CQDs@MIL-125(Ti) photocatalyst can significantly improve the degradation process of TC, and the degradation efficiency can reach 90% within 4 h. The enhancement in the photocatalytic performance is due to the CQDs, which can promote the absorption of visible light and also efficiently accelerate the separation of photogenerated electron–hole pairs. We have also demonstrated that superoxide radicals (·O2−) and holes (h+) play crucial roles in the photocatalytic degradation of TC through capture experiments. The current work provides a new idea for constructing high-efficiency photocatalysts based on MIL-125(Ti).
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2016
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IF 8.328
Yanghe Fu,Long Sun,Huan Yang,Lai Xu,Fumin Zhang,Weidong Zhu
The Ni-doped NH 2 -MIL-125(Ti) catalyst was developed for the photocatalytic aerobic oxidation of aromatic alcohols upon visible light irradiation. The results show that different aromatic alcohols can be effectively transformed to their corresponding aldehydes with almost absolute selectivity using O 2 as the oxidant over Ni-doped NH 2 -MIL-125(Ti) upon visible light irradiation. Compared with the parent catalyst NH 2 -MIL-125(Ti), Ni-doped NH 2 -MIL-125(Ti) exhibits a significantly enhanced photocatalytic activity for the selective oxidation of aromatic alcohols. Preliminary studies indicate that the doping of Ni nanoparticles into NH 2 -MIL-125(Ti) could improve the visible-light harvesting, charge-separation, and electron-transport of the resultant catalyst, leading to the enhanced photocatalytic activity. The current work provides some guidance in the development of MOF-based photocatalysts for organic syntheses.
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Processes
·
2024
·Vol. 12
·期 9
·1879
·
IF 2.8
Huiying Yang,Xiangchao Meng
The conversion of nitrogen (N2) and water (H2O) into NH3by photocatalysis under ambient conditions has been considered an environmentally friendly strategy. However, developing effective catalysts for N2fixation is still challenging. Herein, we report a bimetallic JH Fe, Co/TiO2derived from NH2-MIL-125(Ti) by the fast Joule heating (FJH) method for visible–light–driven catalytic N2fixation. It was found that the photocatalytic N2reduction efficiency of bimetallic FC@TiO2-JH was improved, enabling an NH3yield rate of 110.14 µmol g−1h−1without any sacrificial agents. Furthermore, the rate was higher than those of Fe@TiO2-JH and Co@TiO2-JH, suggesting that the synergistic effect between Fe and Co broke the electronic equilibrium and increased the center of its d-band, enhancing electronic feedback to the antibonding π* orbitals of N2while weakening the bonding energy of N≡N. Meanwhile, the rate was about 2.75 times higher than that of FC@TiO2-TF, which was calcined in a tube furnace. It is assumed that FJH might lead to the formation of lattice defects, leading to localized charge deficiency, enhanced carrier separation, and transport. Thus, doping of Fe and Co synergistically interacted with the defects produced from FJH, facilitating the photocatalytic reduction process. As detected, it had a greater ability to separate hole–electron pairs and transferred electrons to adsorbed N2at faster rates. Our work demonstrates a prospective strategy for designing bimetallic catalysts derived from NH2-MIL-125(Ti) for N2fixation.
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JOURNAL OF HAZARDOUS MATERIALS
·
2022
·
IF 14.224
Youzhou He,Yuwei Tan,Mengyu Song,Qingli Tu,Min Fu,Liangjun Long,Jie Wu,Mengmeng Xu,Xingyan Liu
Photocatalysis technology has been widely adopted to abate typical air pollutants. Nevertheless, developing photocatalysts aimed at improving photocatalytic efficiency is a challenge. Herein, the linker-defect NH 2 -MIL-125(Ti) photocatalyst was synthesized through a convenient one-step heating-stirring method (just adjusting multiple temperatures) to firstly realize efficient photocatalytic performances of NO removal and hydrogen evolution . The optimal sample (named 65-NMIL) with a linker-defect content of 32.08% exhibited a NO removal ratio of 65.49%, which was 37.57% higher than that of pristine NH 2 -MIL-125(Ti), and displayed better H 2 -production activity. Through ESR, it was confirmed that 65-NMIL can generate more •O 2 - and •OH under visible light, and the radical trapping experiment further proved that •O 2 - played a more important role in photocatalytic activity. Moreover, the photocatalytic NO oxidation process was also monitored by in situ DRIFTS , it was found that the defective samples could promote the oxidation of NO and intermediates to the final product (NO 3 - ). On the basis of the above-mentioned photocatalytic experimental results and characterization, a possible mechanism or pathway was proposed and illustrated. This work can provide a new strategy for the subsequent defect engineering for photocatalytic MOFs materials to further solve environmental and energy crises.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2025
·
IF 8.3
Jun-Qing Ye,Bin Cheng,Yunfei Bu,Jun-Feng Qian,Qian Liang,Ming-Yang He,Qun Chen
The development of high-efficiency photocatalysts for water splitting to hydrogen (H 2 ) is crucial for alleviating energy crisis and environmental problems. In this study, a novel type-II ternary heterojunction photocatalyst, CDs/NH 2 -MIL-125 (Ti)/Cu 2 O, was fabricated through the integration of NH 2 -MIL-125 (Ti) with Cu 2 O and carbon dots (CDs), exhibited excellent photocatalytic H 2 production rate of 12817.1 μmol/g/h with apparent quantum efficiency (AQE) of 17.13 % under visible light irradiation. Characterization revealed a uniform and dense structural integration with a high Brunauer-Emmett-Teller (BET) surface area of 275.9 m 2 g −1 and a suitable energy band gap of 2.18 eV. Furthermore, the heterostructures promoted efficient photo-generated carrier separation and enhanced reduction capabilities . Notably, CDs, serving as cocatalysts or electron acceptors, improved visible light utilization and electron migration, significantly boosting H 2 production. Insights from electron spin resonance (ESR) and density functional theory (DFT) calculations supported the migration mechanisms of electrons. This work presents a significant advance in photocatalytic technology for sustainable energy by designing high-performance CDs-modified heterojunction photocatalysts.
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