RSC Advances
·
2019
·Vol. 9
·期 65
·37733-37738
·
IF 3.049
Yanghe Fu,Jieyu Wu,Rongfei Du,Ke Guo,Rui Ma,Fumin Zhang,Weidong Zhu,Maohong Fan
Defect engineering can be a promising approach to improve the photocatalytic performance of metal–organic frameworks (MOFs). Herein, a series of defective NH2-UiO-66(Zr) materials were synthesized via simply controlling the synthesis temperature, with concentrated HCl as the modulator and then these as-prepared samples were used to systematically investigate the effects of their structural defects on photocatalytic CO2 reduction. Remarkably, these MOFs with defects exhibit significantly enhanced activities in photocatalytic CO2 reduction, compared with the material without defects. The defect engineering creates active binding sites and more open frameworks in the MOF, and thus facilitates the photo-induced charge transfer and restrains the recombination of photo-generated charges efficiently. The current work provides an instructive approach to improve the photocatalytic efficiency by taking advantage of the structural defects in MOFs, and could also inspire more work on the design of advanced defective MOFs.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Hao Guo,Likun Luan,Jinde Cai,Xiuling Ji,Haijun Yu,Yuhong Huang
CO 2 activation and conversion by enzymes to produce value-added multi-carbon compounds under mild conditions show significant impact on carbon neutrality. However, the enzyme co-factor NADH is expensive and the regeneration is still challenging for the enzyme reaction process. Inspired by natural photosynthesis, this study successfully developed a biomimetic photocatalyst Ce/TCPP-UiO-66-NH 2 (TCPP: meso-tetrakis (4-carboxyphenyl) porphine) for NADH regeneration and CO 2 activation. Structure analysis and spectra showed that the co-doping of Ce and TCPP reduced the band gap width of UiO-66-NH 2 , improved the separation efficiency of photo-generated carriers, and endowed it with excellent photocatalytic performance. The synthesized biomimetic photocatalyst Ce/TCPP-UiO-66-NH 2 was then applied for NADH regeneration. The regeneration efficiency of NADH can reach up to 95 % after 3 h of light reaction, which was about 1.6 times higher than that of the control group. Ultra-fast femtosecond time-resolved transient absorption (fs-TA) showed that Ce/TCPP-UiO-66-NH 2 possessed the shortest average decay time ( τ ¯ = 1.12 ps), indicating shorter average life-time of carriers after Ce doping, thus suppressing hole-electron recombination. Finally, the key enzyme formate dehydrogenase (FDHPa) for CO 2 activation was immobilized on the membrane, combining with light regeneration of NADH for CO 2 production to formate. The formate yield (3.1 mM) was 16 times higher than that of the control group (0.19 mM). This work provided an effective strategy and efficient photocatalyst for the biomimetic photocatalytic activation of CO 2 to formate, which is an indispensable bridge for the further high-valuable C n compounds production by biocatalysis.
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Processes
·
2023
·Vol. 12
·期 1
·64
·
IF 3.5
Zehui Zhao,Guangmin Ren,Xiangchao Meng,Zizhen Li
In order to achieve efficient photocatalytic N2reduction activity for ammonia synthesis, a photochemical strategy was used in this work. UiO-66 was prepared through the solvothermal method and further loaded with Au nanoparticles (Au NPs) onto the UiO-66 (Zr) framework. The experimental results verified that there were metal–support interactions between Au NPs and UiO-66; this could facilitate charge transfer among Au NPs and UiO-66, which was beneficial to enhance the photocatalytic activity. The best N2fixation effect of Au/UiO-66 with a loading of 1.5 wt% was tested, with a photocatalytic yield of ammonia of 66.28 μmol g−1h−1while maintaining good stability. The present work provides a novel approach to enhancing photocatalytic N2fixation activity by loading NPs onto UiO-66.
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JOURNAL OF MOLECULAR STRUCTURE
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2023
·
IF 3.8
Yongtong Lei,Jinglong Zhao,Haiming Song,Fanhang Yang,Luli Shen,Lijing Zhu,Zhixiang Zeng,Xiaocheng Li,Gang Wang
UiO-66-based metal-organic framework (MOF) materials are a class of porous crystalline materials consisting of Zr metal clusters compounded with organic ligands of terephthalic acid group. In this study, functionalized UiO-66-X ( X =H , NH 2 , (COOH) 2 ) nanoparticles were synthesized. The morphology of UiO-66-X nanoparticles were characterized by SEM, while the crystal structure was analyzed using XRD and TGA . Chemical composition of UiO-66-X nanoparticles were analyzed through TFIR and XPS . The adsorption capacities of UiO-66-X nanoparticles for anionic dye of Congo red (CR), and cationic dyes of methylene blue (MB) and rhodamine B (Rh B) dyes were evaluated. Furthermore, the adsorption mechanisms of UiO-66-X nanoparticles for dyes were analyzed and summarized. Results showed that the adsorption capacities of UiO-66 and UiO-66-NH 2 on CR were 93.05 mg/g and 94.20 mg/g, respectively. In particular, the adsorption capacities of UiO-66-(COOH) 2 on MB and Rh B were significantly increased with the adsorption capacities of 80.66 mg/g and 72.64 mg/g, respectively. Due to the strong π-π effect and hydrogen bonding interactions between UiO-66 and CR dyes. UiO-66-NH 2 has stronger hydrophilicity and has electrostatic interactions , Lewis acid-base interactions and hydrogen bonds with CR. The abundant -COOH groups and higher negative Zeta potential (-23.43 mV) in UiO-66-(COOH) 2 led to strong electrostatic interactions and Lewis acid-base interactions with the cationic dyes MB and Rh B. Therefore, the adsorption performance of UiO-66-(COOH) 2 on cationic dyes was improved.
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CHEMICAL ENGINEERING JOURNAL
·
2018
·
IF 6.735
Shuting Zhuang,Rong Cheng,Jianlong Wang
UiO-66 type metal organic frameworks (MOFs), including UiO-66 and UiO-66-NH 2 , were synthesized, characterized, and applied for the adsorptive removal of diclofenac (DCF) from aqueous solutions. The effect of synthetic conditions (e.g., different linkers and activation temperatures) and adsorptive conditions (e.g., contact time, initial concentration, temperature, and pH) on DCF removal was examined. UiO-66-NH 2 showed a higher adsorption capacity than UiO-66, and the increase of activation temperature can improve the adsorption capacity of UiO-66-NH 2 towards DCF. The adsorption of DCF by UiO-66-NH 2 was endothermic and almost not affected by pH in the range of 4.8–7.7. The adsorption of DCF onto UiO-66 type MOFs conformed to the pseud second-order kinetic model and the Langmuir isothermal model, with adsorption capacity of 357 mg g −1 for UiO-66 and 555 mg g −1 for UiO-66-NH 2 . Electrostatic interaction and H-bonding possibly played a vital role for DCF adsorption. The as-prepared UiO-66 type MOFs were efficient adsorbent for DCF removal from aqueous solution.
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CHEMISTRY OF MATERIALS
·
2019
·
IF 10.159
Shanshan Zeng,Fucong Lyu,Ligang Sun,Yawen Zhan,Fei-Xiang Ma,Jian Lu,Yang Yang Li
In this work, UiO-66-based metal–organic frameworks are investigated as an oxygen reduction reaction (ORR) catalyst for the first time. UiO-66-NO2 is solvothermally grown on the surface of cobalt phthalocyanine-anchored carbon nanotube (CoCNT) surface, serving as an oxygen “pump” to accelerate the oxygen reduction reaction (ORR). The UiO-66-NO2-attached CoCNT (UiO-66-NO2@CoCNT) exhibits superior electrochemical catalytic properties, exceeding the state-of-the-art commercial 20% Pt/C catalyst with more positive half-wave potential (15 mV difference, at 1600 rpm), better stability (no significant degradation for UiO-66-NO2@CoCNT vs 19% degradation for 20% Pt/C after 25 000 s), and higher methanol tolerance. When assembled in a flexible zinc–air battery, the UiO-66-NO2@CoCNT remains a competitive alternative to commercial 20% Pt/C catalyst with comparable power density and excellent flexibility, suggesting its potential in wearable electronic devices. The outstanding performance of UiO-66-NO2@CoCNT composite is closely related to the synergetic effect among the three components: CNT as a conductive backbone, cobalt phthalocyanines as the oxygen reduction catalytic active site, and UiO-66-NO2 as an ideal oxygen adsorption pump (the oxygen diffusion rate is 4.8 times that of 20% Pt/C and 17.7 times that of CoCNT). The synergy between the three components facilitates oxygen adsorption, transfer of adsorbed oxygen molecules, oxygen reduction, and electron conduction.
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CHEMICAL ENGINEERING JOURNAL
·
2019
·
IF 8.355
Zhongguo Wang,Lian Song,Yaquan Wang,Xiong-Fei Zhang,Dandan Hao,Yi Feng,Jianfeng Yao
Composite UiO-66/nanocellulose aerogels with hierarchical pores and low density were prepared through a self-crosslinking method. The nanocellulose acted as the structural skeleton supporting and dispersing the UiO-66 particles. The micropore and accessibility of UiO-66 were well-preserved, making the composite aerogels ideal sorbents for water purification. The composite aerogels demonstrated high adsorption ability towards both anionic methyl orange (71.7 mg g −1 ) and cationic methylene blue (51.8 mg g −1 ). This work holds a promise to rational design and fabrication of MOF monoliths through group linkage.
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JOURNAL OF MEMBRANE SCIENCE
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2018
·
IF 6.578
Xiong-Fei Zhang,Yi Feng,Zhongguo Wang,Mingmin Jia,Jianfeng Yao
Incorporating metal-organic frameworks into cellulose matrix to prepare composite membranes is promising in gas-separation applications. In this study, UiO-66-NH 2 (Zr-based MOF) nanoparticles are wrapped into the densely packed cellulose nanofibrils (CNF-COOH) via a facile vacuum filtration process. The existence of acid-base interactions and electrostatic forces between UiO-66-NH 2 and CNF-COOH renders ideal interfacial morphology. Results show that UiO-66-NH 2 is cross-linked by -COOH groups and well-dispersed in the CNF matrix. The porous UiO-66-NH 2 strengthens the diffusion process of CO 2 molecules, thus elevating the permeation flux and separation factor simultaneously. The optimum separation performance is achieved over CM-1 membrane with a CO 2 permeability of 139 Barrer and a CO 2 /N 2 selectivity ratio of 46.
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CHEMICAL ENGINEERING RESEARCH & DESIGN
·
2019
·
IF 3.073
Kai Wang,Yun Qin,Shuai Quan,Yingjie Zhang,Peng Wang,Heng Liang,Jun Ma,Xi Quan Cheng
With suitable pore size, narrow pore size distribution and charged surface, nanofiltration (NF) membranes show great potential in removing or recovering dyes from effluents of printing and dyeing industries. However, low permeance of commercial nanofiltration membranes hampers their widespread application. Herein, we design a kind of high permeance mixed matrix membranes through layer-by-layer (LbL) self-assembly of polyelectrolytes (PEs). The additional solvent pathways constructed by incorporation of UiO-66, a type of Zr-based metal organic frameworks (MOFs), accelerate the water passing through the membranes; the pure water permeance of UiO-66 incorporated PEs membrane (PEM/UiO-66) achieves at as high as 14.8 L m −2 h −1 bar −1 which is 160% higher than the pristine PEs membrane. Meanwhile, the membrane exhibits 96.3% rejection towards MgSO 4 with molecular weight cut off (MWCO) of 464.2 g mol −1 . The comprehensive separation performance of the mixed matrix membrane outperforms most of state-of-the-art NF membranes fabricated by LbL self-assembly to the best of our knowledge. Most interestingly, the mixed matrix membrane demonstrates solution flux as high as 102 L m −2 h −1 with 99.9% rejection of Congo Red under optimized operation conditions in 240 h continuous operation. Taken together, the UiO-66 incorporated NF membranes show strong promise in removing and recovery of dyes in industrial scale.
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FUEL
·
2017
·
IF 4.601
Xiaotian Zhang,Pengcheng Huang,Aili Liu,Mingyuan Zhu
Owing to the high prices and other shortcomings associated with the existing methods of complex catalyst preparation, we used the UIO-66(Zr) metal–organic frameworks to directly catalyze the oxidative desulfurization (ODS) reaction. The synthesized UIO-66(Zr) was characterized using nitrogen adsorption–desorption isotherm analysis, X-ray diffraction, Fourier transform infrared spectroscopy, transmission electron microscopy, and X-ray photoelectron spectroscopy. Under optimal reaction conditions, the ODS conversion of dibenzothiophene (DBT) reached 100%. This excellent catalytic activity was attributed to the unsaturated coordination of Zr, which may produce beneficial Lewis acid sites.
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FOOD CHEMISTRY
·
2024
·
IF 8.5
Qiyue Zhao,Hong-Man Hou,Gong-Liang Zhang,Hongshun Hao,Bei-wei Zhu,Jingran Bi
Heterocyclic aromatic amines (HAAs), arising as chemical derivatives during the high-temperature culinary treatment of proteinaceous comestibles, exhibit notable carcinogenic potential. In this paper, a composite aerogel (AG D-UiO-66 ) with high-capacity and fast adsorption of HAAs was made with anchoring defective UiO-66 (D-UiO-66) mediated by lauric acid on the backbone of cellulose nanofibers (CNF). AG D-UiO-66 with hierarchical porosity reduced the mass transfer efficiency for the adsorption of HAAs and achieved high adsorption amount (0.84–1.05 μmol/g) and fast adsorption (15 min). The isothermal adsorption model demonstrated that AG D-UiO-66 belonged to a multilayer adsorption mechanism for HAAs. Furthermore, AG D-UiO-66 was successfully used to adsorb 12 HAAs in different food (roasted beef, roasted pork, roasted salmon and marinade) with high recoveries of 94.65%–104.43%. The intrinsic potential of AG D-UiO-66 demonstrated that it could be widely applicable to the adsorption of HAAs in foods.
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高影响因子
MATERIALS SCIENCE IN SEMICONDUCTOR PROCESSING
·
2024
·
IF 4.2
Z.H.A.O.-X.U.A.N. Jiang
In this investigation, UiO-66-NH 2 was effectively synthesized through a solvothermal approach, utilizing benzoic acid and hydrochloric acid (HCl) as modulating agents. This synthesis process intentionally introduced defects mediated by benzoic acid, and the degree of these defects was precisely adjusted by the concentration of HCl. Subsequently, the material underwent a covalent modification process through an amidation reaction, resulting in the attachment of tetrakis (4-carboxyphenyl) porphyrin (TCPP). The results demonstrated a significant improvement in the photocatalytic reduction of Cr(VI), showcasing a 125 % elevation in reduction efficiency as compared to the unmodified UiO-66-NH 2 material serving as the baseline. The performance enhancement is due to the synergistic effect of the defect structure and TCPP modification, which enhances the light absorption, promotes charge transfer and separation, reduces the recombination rate, and improves the adsorption capacity and light absorption efficiency of Cr(VI). This research introduces an innovative approach and a highly effective catalyst, offering a novel solution for modifying metal-organic frameworks (MOFs) and enhancing their photocatalytic performance in the reduction of Cr(VI).
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危险品化学品经营许可证（带存储）