CHEMICAL ENGINEERING JOURNAL
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2023
·
IF 15.1
Sainan Wang,Chao Yuan,Wei Chen,Yifan Niu,Yexi Yan,Fan Li,Hongmei Jiang
A series of CuO@g-C 3 N 4 composites with different contents of g-C 3 N 4 and different morphologies of CuO have been designed and prepared by hydrothermal method and applied to activate peroxymonosulfate (PMS) for the removal 2,4,6-trichlorophenol (2,4,6-TCP). The results showed that 3D spherical shape CuO-1@g-C 3 N 4 -3, being able to activate PMS to produce a large amount of singlet oxygen ( 1 O 2 ), not only had good catalytic performance, but also reduced the dissolution of Cu 2+ . By comparing the morphological characteristics, catalytic performance, free radical species, decomposition rate of PMS and surface properties of three kinds of CuO, the generation mechanism of 1 O 2 and key reasons of CuO for producing 1 O 2 were deeply explored and finally deduced. Besides, under the conditions of initial pH 7.0, catalyst dosage 50 mg·L −1 , PMS dosage 0.3 mmol·L −1 and initial concentration of 2,4,6-TCP 10 mg·L −1 , the removal rate of 2,4,6,-TCP reached 94 % at 25 min in the first cycle, and 85 % in the fifth cycle. When CuO-1@g-C 3 N 4 was applied in actual water samples, 65 % of 2,4,6-TCP was removed in the Yangtze River, and 60 % of 2,4,6-TCP in Xuanwu and Yueya Lake in 40 min. Quenching experiments and electron paramagnetic resonance (EPR) were used to indentify active species during degradation process and the degradation intermediates of 2,4,6-TCP and possible degradation pathways were determined and proposed by high performance liquid chromatography-time of flight-mass spectrometry (HPLC-TOF-MS 2 ). This study shed light on the 1 O 2 generation mechanism of catalyst and provided theoretical basis and guidance for the design of 1 O 2 catalysts rich in non-radical active species.
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JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
·
2023
·Vol. 34
·期 24
·1-17
·
IF 2.8
Fan Yan,Wang Lei,Sun Xueqin,Li Cuili,Liu Jiacheng
A series of UiO-66-NH 2 -CA-Cu/g-C 3 N 4 (UCC 1 /CN x ) heterogeneous photocatalysts were constructed via a facile physical mixing treatment of the covalently post-modified MOF (UiO-66-NH 2 -CA-Cu) and functional materials g-C 3 N 4 . The tetracycline removal by the photocatalysis coupled with persulfate activation were studied under white light irradiation. The optimal UCC 1 /CN 20 photocatalyst showed the best photocatalytic performance, in which 94.0% TC could be efficiently eliminated ( k = 0.08669 min −1 ) within 30 min. The satisfactory degradation performance could be ascribed to the effective separation of photogenerated electron-hole pairs over the heterogeneous binary structure, which were demonstrated by several characteristic technologies including photoluminescence spectra, electrochemical impedance spectroscopy, transient photocurrent response and Bader charge analysis based on density functional theory calculations. Moreover, a possible mechanism behind the photocatalytic degradation was proposed and further affirmed by the quenching experiments and electron spin resonance measurements. Our work may supply a feasible idea for treating wastewater contained organic pollutants based on the heterogeneous photocatalyst.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Xiaoli Jin,Huiqing Wang,Xiongtao Lv,Qing Lan,Teng Ge,Lin Guo,Xin Li,Hongxian Sun,Chenghua Ding,Yuwei Guo,Haiquan Xie,Liqun Ye
The development of bifunctional photocatalysts for enhancing hydrogen (H 2 ) and hydrogen peroxide (H 2 O 2 ) production from water is essential in addressing environmental and energy issues. However, the practical implementation of photocatalytic technology is still constrained by the inadequate separation of photo-generated charge carriers. Herein, potassium (K) atoms are introduced into the interlayers of graphitic carbon nitride (g-C 3 N 4 ) with a hollow hexagonal structure (K-TCN) and are coordinated with N atoms in adjacent layers. The presence of K–N coordination serves as a layer bridge, facilitating the separation of charge carriers. The hollow hexagonal structure reduces the distance over which photogenerated electrons migrate to the surface, thereby enhancing the reaction kinetics. Consequently, the optimized K-TCN exhibits a dramatically improved photocatalytic H 2 (941.6 μmol g −1 h −1 with platinum (Pt) as the cocatalyst) and H 2 O 2 (347.6 μmol g −1 h −1 ) generation as compared to hollow g-C 3 N 4 (TCN) and bulk g-C 3 N 4 nanosheet (CN) without K–N bridge under visible light irradiation. The unique design holds promising potential for developing highly efficient bifunctional photocatalysts towards producing renewable fuels and value-added chemicals.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2023
·
IF 6.2
Shasha Wang,Qing Wang,Wuxin Liu,Yan Wang,Yuli Wei,Shaohua Luo,Pengqing Hou,Yahui Zhang,Shengxue Yan,Xin Liu
Due to the advantages of abundant precursors, simple preparation, and environmental friendliness, nitrogen-doped carbon is considered one of the most potential anodes for potassium ion batteries (PIBs). Here, nitrogen-doped carbon materials (NC-2) were prepared by using secondary exfoliated g-C 3 N 4 as a precursor, combined with sucrose, and subjected to hydrothermal and high-temperature pyrolysis. NC-2 is characterized by high nitrogen content, porous layered structure, and large interlayer spacing. NC-2 used as anode of PIBs shows a high reversible capacity of 261.07 mAh g −1 at 0.1 A g −1 and an impressive rate performance of 153.36 mAh g −1 at 2 A g −1 . The impressive performance of NC-2 can be originated from the porous layered structure and enlarged interlayer spacing promotes the intercalation/deintercalation and the diffusion of K ions , and the defective carbon structure formed after nitrogen doping can supply abundant active sites for K ions. The results show that NC-2 has great potential in the field of PIBs anode.
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CHINESE JOURNAL OF CHEMICAL ENGINEERING
·
2023
·
IF 3.8
Tongming Su,Jundong Meng,Ya Xiao,Liuyun Chen,Hongbing Ji,Zuzeng Qin
Photocatalytic CO 2 reduction to valuable product exhibit promising prospect for solving the energy crisis and the greenhouse effect. Herein, Co-Ti 3 C 2 T x /g-C 3 N 4 (Co-TC/CN) composite with enhanced photocatalytic performance for converting CO 2 to CO and CH 4 was constructed by electrostatic self-assembly method. The close contact interface between Co-Ti 3 C 2 T x and g-C 3 N 4 nanosheets can be used as fast transport channels of photogenerated electrons and effectively promote the separation of photogenerated electrons and holes, and the interface between the Co and Ti 3 C 2 T x might be the active sites for CO 2 adsorption and activation. The optimized Co-Ti 3 C 2 T x /g-C 3 N 4 composite exhibited the highest photocatalytic performance with the CO and CH 4 production of 55.04 μmol·g –1 and 2.29 μmol·g –1 , respectively, which were 7.5 times and 5.9 times than those of g-C 3 N 4 . Furthermore, the stability of g-C 3 N 4 was improved after coupling with Co-Ti 3 C 2 T x .
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ANALYTICAL CHEMISTRY
·
2023
·
IF 7.4
Xingxing Jiang,Shuping Liu,Xianwen Song,Qiang Li,Minghui Yang,Xiang Chen
How to overcome the intrinsic low activity of most oxidase and peroxidase mimics at neutral pH has been extremely challenging. Herein, we represent a chromium-mediated and ligand-dependent strategy to activate the oxidase-like activity of boron-doped g-C3N4 (B-g-C3N4, denoted as BG), aiming at breaking the pH limitation. Cr (III) can be in situ oxidized to Cr (IV) by generated •O2– upon UV light irradiation, which then works as a catalysis mediator to oxidize TMB under a neutral environment. Excitingly, the TMB oxidation can be rationally modulated by ligands on the BG coordinating with chromium. We verify that the PEI-Cr3+ coordination outperformed Cit-PEI-Cr3+ on the oxidase-like activity through a more accelerated electron transfer, unveiled by the Gauss theoretical calculations. This study highlights a paradigm of tuning the coordination environment on nanozyme surface via the ligand engineering strategy for boosting the oxidase-mimicking activity and breaking the pH limitation. Meanwhile, the catalysis-based colorimetric assay for accurate and selective identification of Cr3+ was achieved.
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APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Shasha Wang,Qing Wang,Wuxin Liu,Yuli Wei,Yan Wang,Shaohua Luo,Pengqing Hou,Yahui Zhang,Shengxue Yan,Xin Liu
Carbon materials are still the most widely studied anode materials for potassium ion batteries (PIBs) attributed to their advantages of wide source, controllability, and environmental friendliness. In this paper, a bamboo-like tubular nitrogen-doped carbon material (CNC) was prepared by using g-C 3 N 4 as the precursor and transition metal salt as the catalyst and template. CNC has the advantages of a bamboo-like tubular structure, rich nitrogen content, and large layer spacing. As anode of PIBs, CNC can deliver an impressive initial reversible capacity of 488.6 mAh/g at 0.1 A/g. At a high current density of 1 A/g, CNC still retains a reversible capacity of 291 mAh/g after 1000 cycles. The excellent performance of CNC anode can be due to the porous bamboo-like tubular structure that promotes K ions diffusion and the rich nitrogen content that provides abundant active sites for K ions.
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Materials Advances
·
2023
·Vol. 4
·期 14
·2999-3009
·
IF 5
Xu Jia,Xuetong Xu,Cong Liu,Fuying Wang,Liuxue Zhang,Shuyan Jiao,Genxing Zhu,Guomin Yu,Xiulian Wang
In order to avoid the issues causing weaknesses in the cumene method, a heterojunction catalyst based on Fe(II)-MOF/g-C3N4 was synthesized via in situ synthesis. The combination of Fe(II)-MOF and g-C3N4 was stable. With the synergistic effect of photocatalysis and the Fenton effect, the catalyst could achieve efficient direct hydroxylation of benzene to phenol. The yield and selectivity were 16.4% and 98.8% under the optimum conditions, respectively. And the catalytic activity of the heterojunction still sustained well after 5 reaction cycles. Hence, the explored photocatalysis-self-Fenton system could be applied in the field of direct hydroxylation of benzene to phenol.
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MICROCHEMICAL JOURNAL
·
2023
·
IF 4.8
Qian Wei,Yan Yan,Qingmei Ge,Mao Liu,Nan Jiang,Hang Cong,Jiang-Lin Zhao
A novel photoelectrochemical sensor was constructed by ternary layer-by-layer composites of reduced graphene oxide (rGO), graphitic carbon nitride quantum dots (g-C 3 N 4 QDs), and hemicucurbit[12]uril (HemiQ[12]), on the Indium-Tin Oxide (ITO) piece in sequence. Electrochemical Impedance Spectroscopy (EIS) was employed to confirm the successful assembly of the sandwich electrode, and the functionalization of each layer was explored by comparing of the currents with stepwise coating of the materials to achieve the synergistic enhancement of photoelectrochemical intensity. The application of proposed electrode was achieved by ultrasensitive sensing for chloramphenicol (CAP), which provided a limit of detection low to 0.089 nM, with high selectivity, good reproducibility and stability. The acceptable recoveries for the determination of CAP in real samples of honey and milk illustrated the feasibility of the established analytical method.
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SCIENCE OF THE TOTAL ENVIRONMENT
·
2022
·
IF 10.753
Xue Bai,Juan Shi,Lu Xu,Xin Jin,Xuan Shi,Pengkang Jin
To overcome the shortcomings of homogeneous Fe ion activating peroxymonosulfate (PMS), such as high pH-dependence, limited cycling of Fe(III)/Fe(II) and sludge production, graphite carbon nitride (g-C 3 N 4 ) is chosen as a support for Fe ions, and reduced graphene oxide (rGO) is employed to facilitate the electron transfer process, thereby enhancing catalysis. Herein, a ternary catalyst, Fe-g-C 3 N 4 /rGO, is first applied under lightless condition for PMS activation , which exhibits ideal performance for contaminant mineralization. 82.5 % of the total organic carbon (TOC) in 100 mL of 5 mg/L bis -phenol A (BPA) was removed within 20 min by the optimal catalyst named 30%rFe 0.2 CN, which shows a strong pH adaptability over the range of 3–11 compared with a common Fenton-like system. Moreover, the highly stable Fe-g-C 3 N 4 /rGO/PMS catalytic system resists complex water matrices, especially those with high turbidity . To unveil the mechanism of PMS activation and pollutant degradation , the physicochemical properties of the as-prepared catalysts are comprehensively characterized by multiple techniques. The Fe(III) contained in both the Fe-N group and α-Fe 2 O 3 component of 30%rFe 0.2 CN not only directly reacts with PMS to produce sulfate radicals ( SO 4 − ) and hydroxyl radicals ( OH), but also combines with PMS to form the essential [Fe(III)OOSO 3 ] + active complex, thereby generating superoxide radicals ( O 2 − ) and singlet oxygen ( 1 O 2 ). Among the various reactive oxidizing species, 1 O 2 plays an important role in pollutant removal , which is additionally generated by the C O moiety of the catalyst activating PMS as well as PMS self-oxidation, indicating the dominance of the non-radical pathway in the pollutant degradation process. Due to the advantages of high efficiency, wide pH adaptability and stability, the proposed lightless Fe-g-C 3 N 4 /rGO/PMS catalytic system represents a promising avenue for practical wastewater purification.
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GREEN CHEMISTRY
·
2022
·Vol. 24
·期 24
·9595-9601
·
IF 11.034
Zhenyu Zhang,Anran Li,Haining Na,Fei Liu,Jin Zhu
Fibrillated cellulose with outstanding mechanical strength, biocompatibility, biodegradability and a high specific surface area has attracted widespread attention from researchers. Mechanical fibrillation is the most common preparation method, but a complex pretreatment and high energy consumption are inevitably required. In this study, amino-enriched g-C3N4 as both a relatively weak hydrogen bond donor and a solid base was used in MCF preparation. Almost all kinds of cellulose (without pretreatment) can be directly converted into MCF with a diameter of 200–300 nm with the synergistic action of g-C3N4 and acid (0.02 mol L−1 H2SO4) in 10 min under microwave irradiation. The length of the micro-fibrillated cellulose fiber (MCF) is consistent with the size of the cellulose crystalline region in raw materials. Furthermore, the obtained MCF successfully achieved real-time adsorption of a disperse blue dye and the residue contains a large amount of g-C3N4, which can be used for efficient photocatalytic degradation of rhodamine B. This research, into breaking the hydrogen bonds between fibril bundles by solid–solid interactions rather than mechanical fibrillation, provides a new strategy for MCF preparation.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Sabarinathan Ravichandran,Narayanamoorthy Bhuvanendran,R. Selva Kumar,Putrakumar Balla,Sae Youn Lee,Qian Xu,Huaneng Su
A hybrid catalyst support anchoring a noble metal catalyst could be a promising material for building interfacial bonding between metallic nanostructures and polymer functionalized carbon supports to improve the kinetics of oxygen reduction reaction (ORR). This study successfully prepared a polyhedron nanostructured Pd and MoO 2 -embedded polyaniline-functionalized graphitized carbon nitride (PANI-g-C 3 N 4 ) surface using a chemical reduction method. The Pd–Mo/PANI-g-C 3 N 4 achieved an ORR activity of 0.27 mA µg −1 and 1.14 mA cm −2 at 0.85 V, which were 4.5 times higher than those of commercial 20% Pt/C catalyst (0.06 mA µg −1 and 0.14 mA cm −2 ). In addition, the Pd–Mo/PANI-g-C 3 N 4 retained ∼ 77.5% of its initial mass activity after 10,000 cycles, with only 30 mV half-wave potential reduction. Further, the engineered potential active sites in the catalyst material verified the significant improvement in the ORR activity of the catalyst with increased life-time, and theoretical calculations revealed that the synergistic effect of the catalytic components enhanced the ORR kinetics of the active sites.
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