JOURNAL OF CATALYSIS
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2021
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IF 7.92
Junhui Wang,Shimin Yin,Qinhua Zhang,Fengliang Cao,Yicheng Xing,Qingshan Zhao,Yang Wang,Wengang Xu,Wenting Wu,Mingbo Wu
Polymeric carbon nitride materials show intriguing prospects in numerous light-to-energy conversion applications, but seldom studies focus on their triplet energy transfer, leading to the insufficient lifetime for the photochemical process. Inspired by the porphyrin molecular photocatalyst, single-atom sites (Fe-N 4 ) as triplet sensitizing sites were fabricated in g-C 3 N 4 for the preparation of Fe-g-C 3 N 4 , which processes a long-lived triplet emissive state (τ PH = 4.93 μs). But under realistic condition for the large-scale production of catalyst, single atoms are inevitable to sinter, resulting in the formation of other metal species. Therefore, the photooxidation of 1,5-dihydroxynaphthalene (1,5-DHN) and the photocatalytic E-Z Isomerization of stilbene were selected as the model reactions to evaluate the influence of various Fe species on the triplet energy transfer. It was found that Fe-N 4 sites promote the triplet energy transfer process, while Fe nanoclusters (Fe 0 ) promote the electron transfer and inhibit triplet energy transfer. This finding provides guidance for the rational design of photocatalysts to efficiently improve triplet energy transfer process and its application.
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高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2021
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IF 3.764
Liming Zhao,Lijun Guo,Yuling Tang,Jianfei Zhou,Bi Shi
Research on the rational design of photocatalysts for efficient hexavalent chromium (Cr(VI)) reduction from Cr(VI)-containing wastewater has attracted widespread attention. In this paper, a novel g-C3N4/C/Fe2O3 photocatalyst was successfully synthesized by anchoring g-C3N4 nanosheets onto C/Fe2O3 that was prepared using collagen fiber as the biochar resource following the Fe tanning mechanism to reduce Cr(VI) under artificial solar irradiation. Under the same conditions, the as-prepared g-C3N4/C/Fe2O3 photocatalyst exhibited higher Cr(VI) reduction efficiency than g-C3N4, and the Cr(VI) reduction efficiency increased as Fe content in the g-C3N4/C/Fe2O3 photocatalyst increased. The enhanced photocatalytic performance was primarily ascribed to the formation of an indirect Z-scheme heterojunction between C/Fe2O3 and g-C3N4, which improved the separation efficiency of the photogenerated charge carrier. Furthermore, radical trapping indicated that photoinduced electrons (e–) were the main factor for Cr(VI) reduction. This work provides guidance for high value-added utilization of collagen fiber in constructing efficient light-driven photocatalysts and practical Cr(VI) removal from wastewater.
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CHEMICAL ENGINEERING JOURNAL
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2019
·
IF 8.355
Guomin Li,Bing Wang,Jian Zhang,Rui Wang,Huiling Liu
Through direct thermal condensation of a mixture of Er(NO 3 ) 3 ·5H 2 O and melamine at 550 °C for 2 h, a series of rare earth agent Er (III)-doped mesoporous g-C 3 N 4 (xECN, x = 1,2,3) with different Er content were successfully synthesized. XRD, solid-state 13 C CP/MAS, FT-IR, XPS, UV–Vis DRS, photocurrent, EIS, SEM, TEM, BET and Zeta potentials were used to characterize the phase, morphology, optical and surface properties of xECN photocatalysts. The photo-activities of xECN samples for degradation of Rhodamine B (RhB), tylosin (TYL) and tetracycline (TC) were enhanced compared with those of pure g-C 3 N 4 under the irradiation of simulated solar, and the 2ECN catalyst displayed the optimal degradation rate for all three organic pollutants. The UV–vis results demonstrated that Er doping narrowed the band gap while increasing the light harvesting ability, which improved the photocatalytic activity of g-C 3 N 4 catalyst. The leaching and toxicity tests were conducted with pakchoi seeds and Escherichia coli bacteria, demonstrating that the leaching toxicity of xECN could be ignored. Free radical capture tests were carried out to confirm the main active species for the degradation of RhB under the same experimental condition.
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高影响因子
FUEL
·
2019
·
IF 5.128
Chen Li,Yuefei Song,Xudong Wang,Quan Zhang
Sulfonated titanium dioxide (S-TiO 2 ) was prepared by the grafting of sulfonic groups onto TiO 2 , and doped into the PVDF-g-PSSA as a highly efficient inorganic additive, thus achieving simultaneous improvement of the proton conductivity and anti-fouling property of the synthesized S-TiO 2 /PPSSA proton exchange membrane (PEM). The S-TiO 2 /PPSSA membrane was implemented in microbial fuel cell (MFC) for the first time, and its physicochemical properties and performance in MFC were studied. A new technique of combining Quartz crystal microbalance with dissipation with membrane spin-coated sensors made by a spin coating method was utilized to provide an insight into the anti-fouling property of the prepared membranes. The implementation of Fourier transform infrared spectrometry and X-ray photoelectron spectroscopy demonstrated TiO 2 was successfully introduced into the sulphonic groups. The S-TiO 2 /PPSSA-5.0 membrane has a significant increase in the water uptake (40.9%) and proton conductivity (0.067 S/cm) compared with the PVDF-g-PSSA membrane. QCM-D results indicated that it has better anti-fouling property than pristine membrane and Nafion 117. Moreover, the MFC with the S-TiO 2 /PPSSA-5.0 membrane exhibited a maximum power density of 130.54 mW/m 2 , very close to that of Nafion 117 (132.02 mW/m 2 ), but had the highest COD removal of 91% and least bio-fouling adsorption. These results demonstrate that the blending of sulfonated organic polymers and sulfonated inorganic additives can improve the electrochemical and anti-fouling properties of the composite membranes, which is a new concept for the preparation of PEM suitable for MFC. The S-TiO 2 /PPSSA-5.0 composite PEM is an appropriate candidate separator for the large-scale application of MFCs.
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高影响因子
APPLIED SURFACE SCIENCE
·
2019
·
IF 5.155
Jin Zhang,Yuyang Huang,Tao Nie,Rui Wang,Beibei He,Bo Han,Huanwen Wang,Yongshang Tian,Yansheng Gong
Herein, self-assembly of hierarchical multihole g-C 3 N 4 hexagon with excellent specific surface area (129 m 2 /g) and nitrogen vacancies were accomplished via a one-step polymerization of hydrothermal-treated dicyandiamide and ethylene-diamine-tetra-acetic acid (EDTA). The special chelate structure of EDTA efficiently enlarged a broad visible light response range, and the concentrations of EDTA promoted the self-assembly formation of different surface morphology . The photocatalytic H 2 production rate under visible light for the optimal g-C 3 N 4 hexagon (CN-20E) reaches 5839 μmol·g − 1 ·h − 1 and its apparent quantum efficiency reaches up to 7.3% at 420 nm, which has a 102 times higher for H 2 production rate than that of bulk g-C 3 N 4 (57 μmol·g − 1 ·h − 1 ). Special structure of the multihole hexagon endows them with remarkably visible light absorption, fast separation of photo-induced charge carriers, large surface areas as well as the exposure of potential photocatalytic active sites, thereby dramatically improved the H 2 production property. Moreover, the forming process for the specific structure and the reaction mechanism of the enhanced photocatalytic activity were proposed according to the experimental results and theoretical calculations. This work exhibits a new avenue to rehandle graphitic carbon nitride precursor to build a grafted structure for developing highly efficient g-C 3 N 4 in the practical photocatalytic application.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2019
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IF 8.355
Jiali Zhang,Zhaokun Xiong,Jian Wei,Yonghui Song,Yuezhong Ren,Dongyao Xu,Bo Lai
A cerium-loaded natural zeolite (CZ) was synthesized for catalytic ozonation of penicillin G (PG) in this work. The effects of key factors including Ce loading mass, the initial solution pH, catalyst dosage and ozone dosage were elucidated. Under the optimal conditions: Ce loading mass = 4%, CZ dosage = 2 g/L, ozone dosage = 6 mg/min and the initial solution pH = 4.5, the removal efficiency of PG (50 mg/L in 1 L reactor) reached 99.5% after 15 min, and the total organic carbon (TOC) removal of PG solution reached 21.2% after 2 h. Meanwhile, the results of control experiments indicated that the PG degradation efficiency of CZ/O 3 system was higher than that of O 3 alone system. The CZ catalyst was characterized by TEM, SEM-EDS, XRD, BET and XPS. The results showed that the CZ catalyst retained the high mesopore framework of natural zeolite. Cerium oxide was successfully supported on the zeolite. Then, radical scavenging tests revealed that hydroxyl radical ( OH) and superoxide radical ( O 2 − ) were the dominant reactive oxygen species (ROS) for PG degradation. Furthermore, fifteen species of PG degradation intermediates were found by ultra-high performance liquid chromatography coupled with hybrid quadrupole-orbitrap mass spectrometry (UHPLC/orbitrap-MS) and ion chromatography (IC). Also, two possible PG degradation pathways in the heterogeneous catalytic ozonation systems were proposed and the catalytic mechanism of CZ/O 3 system was analyzed in detail. Finally, the potential toxicity of the intermediates formed during the catalytic ozonation was examined, the toxicity decreased after 60 min. In brief, this study would provide a low-cost and efficient method for removing high concentration PG in solution.
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APPLIED SURFACE SCIENCE
·
2019
·
IF 5.155
Yanhui Dai,Yingjie Gu,Yuyu Bu
Copper element was employed to achieve the interlayer doping and intralayer doping in g-C 3 N 4 (CN). Univalent Cu single atom prefer to dope into the interlayer site of CN to form a steady bridged bond structure. Further increasing the doping amount of Cu, except for the univalent Cu at the interlayer, some divalent Cu single atoms can be doped on the intralayer site of CN to form an unstable but active-catalysis structure. Electrochemical and theoretical calculation results reveal that Cu-interlayer doping can form an energy gradient between the different CN layers to decrease the charge transfer energy barrier between them. More importantly, these interlayer photogenerated electrons will converge on the divalent Cu, a catalysis active site for the photogenerated electrons, inducing more superoxide radicals and high activity. This two-sites modified CN, can mineralize a refractory antibiotic Norfloxacin (NOR) to CO 2 and H 2 O completely under visible light stimulation, and the two-sites co-doping method provides a reference for CN photocatalyst modification to solve the questions of insufficient redox energy and low photons quantum efficiency of CN.
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高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2020
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IF 16.683
Meng Qiao,Xiaofei Wu,Shen Zhao,Ridha Djellabi,Xu Zhao
Due to the complicated chemical nature and toxicity of noble metal-cyanide complexes, the appropriate treatment of wastewaters contaminated with such pollutants is challenging. In this study, the simultaneous decomposition of Ag-cyanide and recovery of precious Ag from Ag-cyanide aqueous solution was investigated using a synergistic peroxymonosulfate (PMS)/g-C 3 N 4 nanosheets system under visible light (λ > 400 nm). The combination of g-C 3 N 4 (1.0 g/L) and PMS (0.5 mM) resulted in higher Ag-cyanide (0.45 mM) decomposition under visible light and Ag recovery efficiencies (74% and 68%, respectively) compared with single PMS oxidation or g-C 3 N 4 photocatalytic oxidation within 150 min. Ag species deposited on g-C 3 N 4 in the form of metallic Ag° and Ag 2 O may also further improve the decomposition of Ag-cyanide complexes. Ag species deposited on g-C 3 N 4 can enhance the separation of electron/hole charges of the photoactive g-C 3 N 4 . Quenching of reactive oxygen species (ROS) experiments and electron spin resonance (ESR) analysis showed the generation of SO 4 ·− , OH, O 2 − , 1 O 2 and e- species in this system, among them O 2 − , 1 O 2 , and e- were the most active species for the decomposition of Ag-cyanide complexes.
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JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY
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2019
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IF 3.261
Hong Yan,Zengwei Zhu,Yumei Long,Weifeng Li
Graphitic carbon nitride (g-C 3 N 4 ) with desired microstructure and chemical functionalities has been drawing considerable interests in terms of their potential applications for environmental treatment and clean energy production. Herein, a novel structure of MoO 3-x ―intercalated g-C 3 N 4 (Mo-g-C 3 N 4 ) and the synthesis strategy were demonstrated by using melamine molybdate as a precursor. The single-source precursor of melamine molybdate ensured the homogeneous mixing between MoO 3-x and g-C 3 N 4 at molecular level. Meanwhile, the strongly chemical interaction between melamine and molybdate promoted the in-situ intercalation of MoO 3-x into g-C 3 N 4 interlayer. The intercalation of MoO 3-x not only improved the visible-light absorption ability, but also facilitated charge separation through interlayer pathway for g-C 3 N 4 . As expected, the Mo-g-C 3 N 4 possesses enhanced activity in the photo-degradation of methyl orange and photo-destruction of Escherichia coli ( E. coli ) bacteria illuminated by visible light. The radicals trap experiments revealed that the holes (h + ) are dominant species in the photocatalysis process over Mo-g-C 3 N 4 . Accordingly, a possible photocatalysis mechanism of pollutants over Mo-g-C 3 N 4 was developed. This study opens up a new way for optimizing microstructure of g-C 3 N 4 -based materials with favorable photocatalytic properties.
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高影响因子
Materials
·
2019
·Vol. 12
·期 23
·3948
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IF 2.972
Lingfang Qiu,Zhiwei Zhou,Mengfan Ma,Ping Li,Jinyong Lu,Yingying Hou,Xiangshu Chen,Shuwang Duo
Novel visible-light responded aluminosilicophosphate-5 (SAPO-5)/g-C3N4composite has been easily constructed by thermal polymerization for the mixture of SAPO-5, NH4Cl, and dicyandiamide. The photocatalytic activity of SAPO-5/g-C3N4is evaluated by degrading RhB (30 mg/L) under visible light illumination (λ > 420 nm). The effects of SAPO-5 incorporation proportion and initial RhB concentration on the photocatalytic performance have been discussed in detail. The optimized SAPO-5/g-C3N4composite shows promising degradation efficiency which is 40.6% higher than that of pure g-C3N4. The degradation rate improves from 0.007 min−1to 0.022 min−1, which is a comparable photocatalytic performance compared with other g-C3N4-based heterojunctions for dye degradation. The migration of photo-induced electrons from g-C3N4to the Al site of SAPO-5 should promote the photo-induced electron-hole pairs separation rate of g-C3N4efficiently. Furthermore, the redox reactions for RhB degradation occur on the photo-induced holes in the g-C3N4and Al sites in SAPO-5, respectively. This achievement not only improves the photocatalytic activity of g-C3N4efficiently, but also broadens the application of SAPOs in the photocatalytic field.Keywords:g-C3N4;SAPO-5;composite;photocatalytic;visible light
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PubMed
高影响因子
RSC Advances
·
2019
·Vol. 9
·期 27
·15196-15204
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IF 3.049
Yun Hong,Dongsen Mao,Rui Wu,Zhe Gao,Tingting Meng,Rongrong Wang,Lin Liu,Jing Miao
DNAzymes have the potential to suppress gene expression through sequence-specific mRNA cleavage and can therefore play an important role in various gene therapies. Hepatitis B virus (HBV) is still one of the most serious liver infections in people around the world and is difficult to treat. We previously designed a 10-23 DNAzyme called DrzBS, which targets HBV S gene expression, but this enzyme depends on exogenous delivery, and so its application has been limited. To overcome this limitation, we have now developed a chitosan-based nanocarrier (chitosan-g-stearic acid, CSO–SA) for intracellular delivery of DrzBS, then compared the inhibition effect of our CSO–SA/DrzBS complex to a common transfection reagent, Lipofectamine™ 2000/DrzBS, on hepatitis B surface antigen expression. The synthesized CSO–SA assembles into micelles in an aqueous solution and exhibits excellent cytoplasmic targeting, and could protect DrzBS from degradation by ribonuclease. CSO–SA/DrzBS showed a higher inhibition rate (IR) than Lipofectamine™ 2000/DrzBS. Moreover, at the same DrzBS concentration (1.2 μmol L−1), the maximum IR of CSO–SA/DrzBS micelles was 2.4-fold that of the Lipofectamine™ 2000/DrzBS complex, and held on for 96 hours. Compared with Lipofectamine™ 2000/DrzBS, CSO–SA/DrzBS achieved a higher HBV inhibition effect. This study demonstrates that CSO–SA micelles can serve as a potential vector for DrzBS and that CSO–SA/DrzBS micelles are a promising application for anti-HBV gene therapy.
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高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2019
·
IF 14.229
Qiaohong Zhu,Bocheng Qiu,Huan Duan,Yeteng Gong,Zengwei Qin,Bin Shen,Mingyang Xing,Jinlong Zhang
Bimetallic phosphides have attracted considerable attention in photocatalytic hydrogen evolution reaction (HER), owing to its thermodynamic feasibility. Most reports attributed the HER activity to the reduction of free energy of protonation (ΔG H* ), however, few revealed the whereabouts of the photo-induced electrons, which makes the mechanism of HER not very clear. Herein, nickel-iron bimetallic phosphide (NiFeP) is designed onto graphitic carbon nitride (NiFeP/g-C 3 N 4 ) for the photocatalytic HER, which exhibits a high hydrogen production of 3.549 mmol g −1 h −1 . It is found that the co-catalyst of NiFeP can not only reduce the ΔG H* , but also make the photogenerated electrons transfer directionally, which play a synergistic role in enhancing the activity of HER. The reduction of ΔG H2O and ΔG H* over NiFeP in HER can be well demonstrated by the density functional theory (DFT) calculations. Furthermore, the localized distribution of electrons on the surface of NiFeP is verified by measuring the lifetime of photo-generated carriers combined with the REDOX experiment. The shortened lifetime τ, decreased τ1 and τ2 of NiFeP/g-C 3 N 4 indicate that the photoexcited electrons of g-C 3 N 4 are directly transferred to the co-catalyst surface, contributing to the worse delocalization capacity of electrons on the ca-catalyst and its easier reactions with protons trapped on the co-catalyst surface. Furthermore, the degradation with peroxymonosulfate (PMS) confirms the photogenerated holes over 5NiFeP/g-C 3 N 4 are mainly concentrated on the surface of g-C 3 N 4 to decompose H 2 O for the generation of OH, while the photogenerated electrons are directed to the NiFeP to react with the neighboring PMS or protons to form SO 4 − or H 2 . Besides, the density of state intensity (DOS) also confirms the photogenerated electron migration pathway at the metal-semiconductor (NiFeP-g-C 3 N 4 ) interface. Our research clarifies the mechanism of bimetallic phosphides co-catalytic HER system, which will provide theoretical guidance for the design and preparation of multi-metallic center photocatalytic system with a higher HER activity in the future.
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