JOURNAL OF MEMBRANE SCIENCE
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2023
·
IF 9.5
Yangyang Dai,Zhenhua Niu,Tian Fang,Yuanyuan Wang,Suyue Zhong,Peng Mu,Jian Li
The structural advantages of the membrane material itself are critical to the membrane separation performance. Two-dimensional (2D) graphitic carbon nitride (g-C 3 N 4 ) nanosheets can achieve minimal mass-transfer barrier and high gas sieving performance due to their ultra-thin thickness, inherent surface porosity and abundance of amine groups. However, the 2D g-C 3 N 4 nanosheets are prone to stacking during the self-assembly process, which reduces the membrane permeability. Based on this line, herein, we proposed a concept of construction of 1D-2D intercalated network supported ionic liquid membrane composed by one-dimensional (1D) carboxymethylcellulose ( CMC ) and g-C 3 N 4 nanosheets to overcome the low permeability of 2D graphitic carbon nitride membrane in separating CO 2 /N 2 and CO 2 /CH 4 . The as-prepared 1D-2D intercalated network supported ionic liquid gas separation membrane exhibits superior CO 2 permeance of 953.96 GPU, CO 2 /N 2 selectivity of 55.46 in separation of CO 2 /N 2 , and CO 2 permeance of 854.00 GPU, CO 2 /CH 4 selectivity of 50.62 in separation of CO 2 /CH 4 . In addition, the resulting CMC@g-C 3 N 4 /IL membrane has excellent durability. After 120 h of testing, it still has outstanding separation performance. In short, this concept in this study provides an effective modulation of molecular sieving of g-C 3 N 4 membrane for high-efficiency CO 2 capture by combination of the advantages of the 1D (CMC) and 2D (g-C 3 N 4 ) materials.
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Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Siao Li,Weisong Yan,Changyi Yang,Yanshu Zhu,Ying Liu,Yaohua Gu,Zhiqiang Wu,Keren Shi,Huiqin Yao
Acridine , as a nitrogen heterocyclic pollutant, poses a huge ecological and human health hazard, and its efficient degradation is one of the top tasks. A novel photo-enzyme-coupled catalytic system was constructed by coupling horseradish peroxidase (HRP) with graphite carbon nitride (g-C 3 N 4 ) through a simple inorganic hybridization process. The obtained g-C 3 N 4 /HRP nanoflowers not only increase the enzyme loading capacity and enzyme activity , but also promote the efficient separation of carriers. More importantly, the H 2 O 2 generated by g-C 3 N 4 directly participates in the redox cycle reaction of HRP, inducing photo-enzyme synergistic catalysis. Therefore, compared to HRP nanoflowers and g-C 3 N 4 nanoflowers, g-C 3 N 4 /HRP nanoflowers exhibited higher catalytic efficiency for the degradation of acridine. Thus, the photo-enzyme coupled catalyst proposed in this study provides a promising platform for the degradation of acridine pollutants by combining enzymes with photocatalysts through inorganic hybridization.
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ACS Catalysis
·
2023
·
IF 12.9
Qian Zhang,Mingzi Sun,Chen-Yue Yuan,Qi-Wen Sun,Bolong Huang,Hao Dong,Ya-Wen Zhang
Constructing abundant surface/interface structures has significant impacts on improving the performance of electrochemical CO2 reduction reaction (CO2RR) catalysts. For developing high-performance CO2RR catalysts, herein we report a 0D/2D heterojunction structure of SnO2 nanodots (∼2 nm) confined on graphitic carbon nitride (g-C3N4) nanosheets for promoting the conversion of CO2 to formate. Experimental and theoretical studies demonstrate that the abundant N-coordinating sites of g-C3N4 and highly distributed SnO2 nanodots synergistically lead to strong metal oxide–support interactions, and the substantial heterojunction interface in SnO2/g-C3N4 has induced efficient electron transfer from electron-rich g-C3N4 to SnO2 mainly through p–p orbital couplings. As a result, the SnO2/g-C3N4 heterojunction provides superior activity and stability for the conversion of CO2RR to formate, with a Faradic efficiency of 91.7% at −0.88 V vs RHE. Moreover, the proposed 0D/2D heterojunction strategy was extended to In2O3/g-C3N4, supplying a universal strategy to achieve efficient hybrid catalysts for CO2RR in the production of high-value chemicals.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Shanshan Song,Miao Yang,Fei He,Xiao Zhang,Yijun Gao,Baichao An,He Ding,Shili Gai,Piaoping Yang
Nanozyme-based synergistic catalytic therapies for tumors have attracted extensive research attention. However, the unsatisfactory efficiency and negative impact of the tumor microenvironment (TME) hinder its clinical applications. In this study, we provide an easy method to prepare transition metals loaded onto pyrrolic nitrogen-rich g-C 3 N 4 (PN-g-C 3 N 4 ) for forming metal-N4 sites. This N-rich material effectively transfers electrons from g-C 3 N 4 to metal-N4 sites, promotes the oxidation–reduction reaction of metals with different valence states, and improves material reusability. Under TME conditions, copper ions loaded onto PN-g-C 3 N 4 (Cu-PN-g-C 3 N 4 , CPC) can produce ·OH through a Fenton-like reaction for tumor inhibition. This Fenton-like reaction and tumor cell inhibition can be improved further by a photodynamic effect caused by light irradiation. We introduced upconversion nanoparticles (UCNPs) into CPC to obtain nano-enzymes (UCNPs@Cu-PN-g-C 3 N 4 , UCPC) for effectively penetrating the tissue, which emits light corresponding to the UV absorption region of CPC when excited with 980 nm near-infrared (NIR) light. The nanoplatform can reduce H 2 O 2 concentration upon exposure to NIR light; this induces an increase in dissolved oxygen content and produces a higher supply of reactive oxygen species (ROS) for destroying tumor cells. Owing to the narrow bandgap (1.92 eV) of UCPC under 980 light irradiation, even under the condition of hypoxia, the excited electrons in the conduction band can reduce insoluble O 2 through a single electron transfer process, thus effectively generating O 2 •– . Nanoenzyme materials with catalase properties produce three types of ROS (·OH, O 2 •– and 1 O 2 ) when realizing chemodynamic and photodynamic therapies. An excellent therapeutic effect was established by killing cells in vitro and the tumor-inhibiting effect in vivo , proving that the prepared nanoenzymes have an effective therapeutic effect and that the endogenous synergistic treatment of multiple treatment technologies can be realized.
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高影响因子
Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Peng Chai,Chunjia Luo,Jincui Gu,Fan Yu,Min Chao,Xi Chen,Luke Yan
Integrating photocatalytic degradation and membrane separation is a crucial approach to water purification . Here, inspired by Euplectella aspergillum, we presented an electrospinning fibrous membrane containing polyacrylonitrile (PAN), graphitic carbon nitride (g-C 3 N 4 ) particles, and polyvinylpyrrolidone (PVP). The g-C 3 N 4 particles undertook the task of photocatalytic degradation for various contaminants. The PVP molecules assumed the role of pore-forming agent for providing additional channels for high-throughput wastewater purification. Furthermore, the micro/nano porous structure of the PPAN@g-C 3 N 4 fibers promoted the exposure of the photocatalytic active center of the g-C 3 N 4 particles, improving the light absorption capacity and enhancing photocatalytic performance. Hence, the prepared PPAN@g-C 3 N 4 fibrous membrane possessed excellent separation properties for the oil/water mixture (53,555 ± 3241 L m −2 h −1 bar −1 ) and oil-in-water emulsion (103,689 ± 13,286 L m −2 h −1 bar −1 ), and maintained its initial separation performance after cyclic separation. Moreover, the membrane showed excellent photocatalytic performance for different pollutants, among which the photocatalytic efficiency of RhB , MB , and MG was about 100 %. After 7 consecutive photocatalytic degradation of RhB, the efficiency remained above 95 %. Meanwhile, the antibacterial efficiency was more than 87 %. The combination of high-throughput separation performance and excellent catalytic performance exemplifies its potential attractiveness for practical wastewater purification.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2023
·
IF 6.2
Xiaoxi Yu,Xiaocui Wu,Fang Guo,Jingping Liu,Qingshan Zhao
As a promising advanced oxidation process , photo-assisted peroxymonosulfate (PMS) activation for wastewater treatment has attracted widespread attentions. However, rational design of synergetic and recyclable catalysts for PMS photo-activation remains a big challenge. In this study, a carbon layer-coated amorphous CoO x supported on graphitic carbon nitride (CoO x @C/g-C 3 N 4 ) composite was fabricated to drive visible-light-assisted activation of PMS for efficient organic pollutant degradation. Amorphous CoO x nanoparticles were in-situ grown on two-dimensional g-C 3 N 4 substrate, among which a carbon layer serves as a high-speed electron transmission channel, facilitating the separation of photogenerated electron-hole pairs and accelerating the Co 3+ /Co 2+ redox cycle. Simultaneously, the carbon layer provides a protective film to suppress Co leaching, thereby improving the catalytic activity and reusability. Owing to the unique heterostructure and synergetic effect, the optimized 6% CoO x @C/g-C 3 N 4 composite exhibits superior catalytic efficiency and excellent cycling stability towards the degradation of various organic pollutants, which displays nearly 100% elimination of tetracycline (TC) within 80 mins. The h + , SO 4 •- and •OH are determined as the main contributors in the visible light-assisted PMS activation system, and the possible catalytic mechanism is also proposed. This work demonstrates a feasible strategy for constructing synergetic and effective photo-activation PMS catalysts for water remediation.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2023
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IF 22.1
Junpeng Yue,Hanpei Yang,Chen Liu,Qiang Zhang,Yanhui Ao
A new strategy to realize efficient removal of organics from water through photo-self-Fenton was investigated. Characterizations and calculations demonstrated that a novel twin carbon nitride with abundant surficial N-defects and compressed π-π layer stacking can be constructed by thermal polymerization of urea under suitable basicity. Synergistically, the twins exhibited an in-situ H 2 O 2 producing at a rate as high as 26.36 mM h −1 g −1 at 420 nm that exceeded most reported C 3 N 4 , and their mineralization rates for Tetracycline Hydrochloride, Bisphenol A , Ciprofloxacin, and Rhodamine B reached 8.8, 15.2, 9.1, and 13 times higher than that of pristine C 3 N 4 . It is concluded that enriching both of photogenerated electrons and molecular oxygens on specific sites plays a crucial role during photocatalysis-self-Fenton process. Particular attentions have to be paid to build structures achieving one and two-electron reduction of O 2 , and activation of H 2 O 2 to •OH simultaneously.
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CHEMICAL ENGINEERING JOURNAL
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2023
·
IF 15.1
Guiyang Yu,Ke Gong,Chuanwang Xing,Lan Hu,Haibin Huang,Lejie Gao,Debao Wang,Xiyou Li
Organic semiconductor under photoexcitation could generate abundant strong-binding Frenkel excitons and inevitably suffer from low dissociation efficiency (<1%) and poor mobility ability, which severely suppresses the efficient utilization of photogenerated charges and corresponding activity. Herein, a dual P-doping strategy is proposed in bay and corner sites implanted polymeric carbon nitride (PCN-D) for visible-driven H 2 O 2 production. The dual P doping breaks localized electron state around original symmetric heptazine units and weakens the binding energy between electrons and holes, increasing dissociation efficiency to reach 11.9% with 20-fold improvement. In addition, the conductivity ability of PCN-D, including formed carrier charge concentration and mobility, achieves 13-fold and 7-fold improvement, which facilitates the charge transfer and separation. The proposed dual doped-P-site strategy, with the blessing of porous structure, provides plentiful active center for effective adsorption and activation of O 2 molecule, further accelerating reaction progress and achieving six-times increase of photocatalytic H 2 O 2 production rate. This work provides in-depth insight into the importance of dual P-doping to optimize kinetic behavior of photogenerated charges and opens an avenue to the multiscale doping-modulation of semiconductor with high efficiency solar energy conversion.
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OPTICAL MATERIALS
·
2023
·
IF 3.9
Jia Li,Jianfeng Zheng,Xingmin Liu,Yatao Yang,Xiaojin Han,Zhanggen Huang
Photoelectrochemical reduction of CO 2 with H 2 O into syngas (H 2 /CO) is considered as an important platform to organic chemicals, which can effectively alleviate the greenhouse effect and energy dependence. We synthesized SnO/g-C 3 N 4 p-n junction catalyst with matched energy band, which shows enhanced light absorption performance and photogenerated charge separation efficiency. The M − S plots verified the successful construction of p-n type heterojunctions , and the investigations of LSV , EIS , PL and transient photocurrents test indicate that the recombination rate of charge is well inhibited by the design of p-n heterojunction. In this work, the syngas derived from PEC reduction of CO 2 and H 2 O is achieved by the SnO/g-C 3 N 4 photocathode with a total FE of 70% at an external bias of −1.5 V. In addition, the H 2 /CO molar ratio can be tuned from 1.5 to 10 by controlling the applied voltage. The study may inspire a new thought for the design of high-performance photoelectric catalyst and a promising strategy for PEC CO 2 reduction to valuable carbon-based compounds.
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CHEMISTRY-A EUROPEAN JOURNAL
·
2018
·Vol. 25
·期 9
·2330-2336
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IF 5.16
Jing Liu,Xiuxia Zhao,Peng Jing,Wei Shi,Peng Cheng
Graphical Green hybrid : A Z-Scheme system, g-C 3 N 4 /α-Fe 2 O 3 , was synthesized by a MOF-derived template method. The optimized system shows excellent photocatalytic hydrogen evolution performance with visible light response. As one of the most efficient systems for photocatalytic hydrogen evolution, the Z-Scheme system, consisting of different semiconductors with a reversible donor–acceptor pair, has attracted great attention. Considering the non-toxicity and low cost of photocatalysts, a series of g-C 3 N 4 /α-Fe 2 O 3 hybrids were rationally constructed based on the Z-Scheme mechanism for the first time, using a metal-organic framework template approach that can fine tune the compositions and properties of the hybrids. An optimized hybrid, g-C 3 N 4 /α-Fe 2 O 3 -2, exhibited prominent photocatalytic water splitting performance with a visible light response. Under irradiation of visible light ( λ >420 nm), the hybrid shows a high durability and superior hydrogen production rate of 2066.2 μmol g −1 h −1 from water splitting, which is approximately three times greater than that of bulk g-C 3 N 4 because of the effective separation of photo-excited charge carriers by two narrow band gap semiconductors, tightly coupled with the Z-Scheme structural feature.
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JOURNAL OF MATERIALS SCIENCE
·
2019
·Vol. 54
·期 10
·7834-7849
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IF 3.442
Dong Xuejun,Wu Keliang,Zhu Weifang,Wu Pengcheng,Hou Juan,Wang Zhaoxiong,Li Ran,Wu Jianning,Liu Zhiyong,Guo Xuhong
As a strong oxidizing pollutant, NO 2 can cause fire or even explosion. People living in atmosphere containing NO 2 for a long time will significantly affects human health. In this work, we developed a Schottky heterojunction sensor modified by g-C 3 N 4 quantum dots (g-C 3 N 4 QDs) and rGO deposited on TiO 2 nanotubes (TNTs) arrays. This sensor showed high response and extremely fast response/recovery time as well as excellent detection of ppb level of NO 2 at room temperature. TNTs were obtained using a one-step anodic oxidation process. TNTs were modified with g-C 3 N 4 QDs and rGO using quasi -CVD method and cyclic voltammetry during in situ electrodeposition, respectively. TNTs/g-C 3 N 4 QDs/rGO Schottky heterojunction sensor exhibited high sensitivity to 10 ppm of NO 2 (response equal to 15982) at room temperature. Below 15 ppb, sensing response also can reach 127. Sensor response was very fast and increased to 15982 in just 2 s when exposed to 10 ppm of NO 2 after which it recovers 90% within 1.16 s. This work clarified the influence of abundant oxygen vacancies (VO · ) in TNTs and photogenerated electrons on TNTs/g-C 3 N 4 QDs/rGO nanostructures as well as their sensing performances. Our experimental details demonstrated that Schottky barrier was established between TNTs and rGO, which was very beneficial for ppb-level NO 2 detection at room temperature.
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CATALYSIS TODAY
·
2019
·
IF 4.888
Lina Chi,Yingjia Qian,Junqiu Guo,Xinze Wang,Hamidreza Arandiyan,Zheng Jiang
Membrane fouling due to superhydropobicity of polytetrafluoroethylene ultrafiltration membranes (PTFE UFMs) represents a grand challenge for their practical applications in diverse water treatment industries. Surface immobilisation of hydrophilic and chemically stable inorganic metal oxides (TiO 2 , ZrO 2 , etc) has been developed to improve hydrophilicity of the PTFE UFMs, though they still suffer from expensive and repeating regenerations once fouled. To address such issues, we strive to firmly immobilize g-C 3 N 4 modified TiO 2 (g-C 3 N 4 /TiO 2 , hereafter CNTO) onto PTFE UFM via a facile plasma-enhanced surface graft technique using polyacrylic acid (PAA) as a bridging agent. As reported here, the obtained CNTO/PAA/PTFE UFM shows much smaller surface water contact angle (WCA) of 62.3° than that of bare PTFE UFM(115.8°), leading to enhanced water flux of 830 L m −2 h -1 in the initial ultrafiltration of modelled waste-water containing methylene blue (MB). The CNTO/PAA/PTFE UFM is highly resistant to fouling in the prolonged filtration of 1000 mg/L bovine serum albumin (BSA) solution, while the fouled CNTO/PAA/PTFE UFM is able to regenerate rapidly under either UV or visible-light irradiation. The enhanced performance of the novel CNTO/PAA/PTFE UFM is reasonably attributed to its high wettability and robust photocatalytic activity of the g-C 3 N 4 /TiO 2 coating that follows different self-cleaning mechanisms under UV and visible light irradiations.
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