CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Xingyu Zhan,Yunxiong Zeng,Zhilong Zhang,Yingchun Xia,Jingcai Xu,Bo Hong,Xinqing Wang
Antibiotic pollution has potential toxicities to living organisms and the ecological environment and draws great concern of researchers. Photocatalytic degradation of antibiotics by g-C 3 N 4 shows an unsatisfied activity due to the low utilization efficiency of photogenerated electrons and severe charge recombination. A main reason is the neglect of the utilization of electrons at the depth of the material surface. Herein, we report local microenvironment rearranged g-C 3 N 4 (V C, N -CN 6 ) with intrinsic gradient concentration nitrogen (V N ) and carbon vacancy (V C ) via KBH 4 etching followed by water oxidation, enabling a complete photocatalytic degradation (≥99.6%) of TC within 3 min under visible light. This photoactivity has a universality, and can completely visible-light photodegrade sulfadiazine and ciprofloxacin in a short time. Such an extraordinary activity is ascribed to cooperation between gradient V N modulating utilization of internal electron and V C enhancing reactive species generation. Additionally, photodegraded pathways, intermediates, and risks of TC photocatalytic degradation were elucidated by the HPLC-MS and quantitative structure-effect relationship mathematical model. This work enriches the toolbox to engineer the local microenvironment of photocatalysts to upgrade the utilization of internal photoexcited electrons and heighten TC photocatalytic degradation efficiency.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2023
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IF 9.9
Yan Dong,Sheng Liu,Wenjing Deng,Hao Zhang,Guangyi Liu,Xiaolei Wang
Heteroatom doping is a possible way to regulate the catalytic capability of electrocatalysts for hydrogen evolution reaction (HER). This work focuses on the development of bimetallic Cobalt-Iron sulfide ultrathin nanosheets supported on the graphitic carbon nitride (g-C 3 N 4 ) catalyst as efficient HER electrocatalysts (CoS 2 /FeS 2 /CN) with good stability at wide pH value. The ultrathin nanosheet exposes more active sites and enhances the catalyst activity. Electrochemical experiments demonstrate that adding g-C 3 N 4 and Fe to CoS 2 increases its catalytic activity and stability. Furthermore, g-C 3 N 4 and Fe co-doped with CoS 2 can modulate electronic structures on the interface. The CoS 2 /FeS 2 /CN exhibits outstanding HER performance, reaching a current density of 10 mA cm −2 with overpotentials of only 76.5 mV in an acidic solution and 175.6 mV in an alkaline solution. It also demonstrates exceptional durability, superior to commercial platinum/carbon catalysts. This work introduces a promising approach for designing low-cost, high-performance HER electrocatalysts with a wide pH range.
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Journal of the Taiwan Institute of Chemical Engineers
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2023
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IF 5.7
Yanxi Zhao,Shiyan Huang,Chengchao Liu,Yuhua Zhang,Longsheng Wang,Aihua lin,Jinlin Li
Background The design and synthesis of catalysts with high stability, activity and selectivity in Fischer–Tropsch synthesis (FTS) have been attracting extensive research attention. Maintaining high catalytic stability and activity is the best strategy for improving the catalyst efficiency and economic benefits. Methods In this study, graphitic carbon nitride (g-C 3 N 4 )-coated SBA-15 was utilised as a support material to prepare cobalt-based FTS catalysts. The catalysts coated with g-C 3 N 4 were studied via TEM, XPS, XRD, H 2 -TPR, TG, N 2 adsorption–desorption, and tested in a fixed-bed reactor. Significant findings The catalysts coated with g-C 3 N 4 were considerably more stable than the Co/SBA-15 catalyst without g-C 3 N 4 coating during a 100 h test period. Furthermore, the CO-conversion performance of the Co/SBA-15 catalyst decreased continuously. Notably, the activity of the Co/ [email protected] 3 N 4 catalyst with a low g-C 3 N 4 loading was higher than that of the Co/SBA-15@1C 3 N 4 catalyst with a relatively high g-C 3 N 4 loading. g-C 3 N 4 can significantly strengthen the interaction between the cobalt species and the support, thereby increasing the catalyst stability. Therefore, a highly stable catalyst with good activity can be achieved by employing a small amount of g-C 3 N 4 for surface modification. The results highlight the effectiveness of the proposed strategy for preparing highly stable, cobalt-based catalysts with good activity.
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NEW JOURNAL OF CHEMISTRY
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2023
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IF 3.3
Weilong Zhang,Xian Li,Huan Cheng,Jie Yang,Jumei Li
Herein, hollow hZrO2/g-C3N4 composite photocatalysts were successfully fabricated using polymethylacrylic acid (PMAA) nanospheres as sacrificial templates via reflux-precipitation polymerization and subsequent ZrO2 layer coating by sol–gel method over PMAA nanospheres, calcining process, and forming composites with g-C3N4 in sequence. The formation mechanism of the unique composites was proved by FESEM, TEM, XPS, XRD, and EDX mapping characterizations. The photodegradation tests of methylene blue (MB) and ciprofloxacin (CIP) were used to investigate the photocatalytic activity. The results revealed that hZrO2/g-C3N4 exhibited significantly boosted photocatalytic activity for degrading 99.7% methylene blue and 81.5% ciprofloxacin in 120 min under simulated sunlight irradiation (Xe lamp, 500 W), which was much better than that of hZrO2 (42.1% for MB and 19.1% for CIP). The enhanced performance is presumably attributed to the synergetic interaction of the two components and the efficient separation of the photoproduced electron–hole pairs between ZrO2 and g-C3N4, which was verified using photocurrent and EIS characterizations. On the basis of the scavenging studies of free radicals (e−, h+, ˙O2−, and ˙OH), the mechanism of the boosted photocatalytic activity was proposed. More significantly, the composites presented excellent reusability confirmed by cyclic photocatalytic degradation experiments, which is crucial for the sustainable and green applications of photocatalysts.
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Materials
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2023
·Vol. 16
·期 14
·4979
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IF 3.4
Wen Zhong,Jiazhi Dong,Siqiang Chen,Zhe Tong
The synergistic effect of different types of solid particles in liquid lubricants is of great interest. In this work, g-C3N4nanosheets were initially prepared using a calcination method and then as-prepared, and h-BN were used as lubricating additives to the white oil. A comparison between the mixed additives and the single g-C3N4or h-BN additives revealed that the base oil with the addition of g-C3N4and h-BN showed the best lubricating properties. The results show a 12.3% reduction in friction coefficient, resulting in a 68.6% reduction in wear rate compared to the white oil when filled with 0.5 wt% g-C3N4and h-BN (1:1 by weight). Moreover, the addition of g-C3N4and h-BN improves the high-temperature lubrication properties of the white oil. However, the friction coefficient and wear rate increase with increasing oil temperature. The large contact area between g-C3N4and its sliding counterpart and the strong adhesive force between h-BN and its sliding counterpart improve the film formation efficiency, leading to enhanced tribological properties under oil lubrication conditions.
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DESALINATION
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2023
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IF 9.9
He Zhang,Wenmei Luo,Yuping Du,Hao Shi,Guangyong Zeng,Xinxing Yan,Xiaoke Li
Although solar steam generation (SSG) technology has shown promising advantages in the desalination of seawater, the treatment of organic pollutants in wastewater using SSG technology remains a challenge. Furthermore, the efficacy of evaporation materials is often hindered by the presence of organic pollutants, thereby limiting their practical application in the desalination of high-salinity wastewater. To address this issue, a synergistic approach combining photoevaporation and photocatalysis has been proposed as a potential solution. In this study, a novel rGO/MWCNTs aerogel (GMA) modified by photocatalyst g-C 3 N 4 was fabricated by hydrothermal synthesis in the integrated treatment of unconventional waters. At one solar radiation (1 kW·m −2 ), GMA achieved an evaporation rate of 2.07 kg·m −2 ·h −1 and a remarkable solar evaporation efficiency of 92.7 %. In addition, GMA demonstrated excellent desalination performance with over 98 % removal of waste metal ions from seawater and brackish water after desalination. First applied aerogel to the lithium chloride wastewater evaporation and concentration, achieving the concentration of lithium chloride wastewater from 700 mg/L to 5.18 g/L. Additionally, the coordinated photocatalysis of g-C 3 N 4 and rGO resulted in catalytic degradation rates of RhB and TB up to 91.6 % and 87.9 %, respectively. This study provides a new idea for SSG technology in high-salinity wastewater treatment .
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2023
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IF 9.9
Xulong Pang,Yong Li,Xiaofu Wu,Bingmiao Zhang,Ming Hao,Yan Zhu,Yi Zhang,Chuanjiang Qin,Hongmei Zhan,Chuanli Qin
It is highly desirable to explore functionalized polymer semiconductor/g-C 3 N 4 heterojunction photocatalysts with the tight interfacial connection for promoting the photogenerated electron-hole pair separation, improving the hydrophilicity , extending the visible light response and achieving the efficient visible light-driven H 2 evolution. Herein, we synthesized novel poly[9,9-bis(3-ethyl phosphate propyl)fluorene- alt -benzothiadiazole] (PPFBT) with a phosphate ester on every repeating unit by the Suzuki polymerization and then fabricated PPFBT/hydroxylated g-C 3 N 4 (PPFBT/CN-OH) heterojunctions via a surface hydroxyl-induced assembly process. The ratio-optimized 5PPFBT/CN-OH shows the hydrogen evolution activity of 2662.4 μmol·g −1 ·h −1 , an 11.1-time enhancement compared to CN-OH. The improved photocatalytic activity is mainly attributed to the enhanced electron-hole pair separation due to the tight interfacial connection by hydrogen bond (P=O…H-O) and N…S interactions between PPFBT and CN-OH. It is verified that abundant phosphate ester groups of PPFBT improve the hydrophilicity and form coordination bonds with platinum (P=O:Pt) as a cocatalyst to facilitate water splitting for H 2 evolution. It is also confirmed that the enhanced electron-hole pair separation is mainly dependent on the excited high-energy level electron transfer from CN-OH to PPFBT. This work provides a rational molecular design strategy for constructing efficient functionalized polymer semiconductor/g-C 3 N 4 heterojunctions for sunlight-driven H 2 evolution.
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Catalysis Science & Technology
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2023
·Vol. 13
·期 20
·5892-5901
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IF 5
Jifang Cui,Zhihao Yu,Linhao Sun,Ming Zhang,Mengyan Guo,Jian Xiong,Yina Qiao,Rui Zhang,Xuebin Lu
Selective photocatalytic oxidation rather than mineralisation is essential for the catalytic valorisation of biomass, which requires precise control of the generation of reactive oxygen species via the rational construction of heterogeneous junctions. In this paper, CdIn2S4/g-C3N4 (CIS/CNNS) heterojunctions were constructed by a microwave-assisted method and used for selective photocatalytic oxidation of 5-hydroxymethylfurfural (HMF) to 2,5-diformylfuran (DFF), a key intermediate for fine chemical synthesis and an important furan-based polymer monomer. According to the electron transfer mechanism of the heterojunctions, the effective separation of charges and holes led to a significant enhancement of the utilization efficiency of photogenerated electrons (PGEs). Specifically, the valence band (VB) potential of the constructed heterojunctions did not reach the oxidation potential of ˙OH/OH−, which avoided the massive generation of strongly oxidizing active species ˙OH and thus increased the reaction selectivity. Under visible light irradiation, 65.2% HMF conversion and 91.5% DFF selectivity could be achieved over CIS/CNNS, with a product yield 3.26 times higher than monomeric CdlIn2S4 and 4.2 times higher than monomeric CNNS. The radical quenching experiments verified that ˙O2− was the predominant active species in the reaction process, and the ˙O2− signal of the composite was significantly enhanced in the ESR characterization, achieving highly selective conversion of HMF to DFF.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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IF 8.6
Wenyuan Lu,Lanyue Qi,Dachang Dong,Xianbao Shen,Lijie Xu,Ying Zhang,Xiang Mei,Weichuan Qiao,Xuewen Guo,Yuwei Pan
In this study, g-C 3 N 4 catalysts were prepared from six different precursors including urea, melamine and its hydrochloride, dicyandiamide, thiourea, trithiocyanuric acid to compare their photocatalytic performance and the activation of three commonly seen peroxides, i.e., H 2 O 2 , peroxymonosulfate (PMS), and peroxydisulfate (PDS) under visible light irradiation. The structural and photoelectric properties were analyzed systematically. Results showed that the g-C 3 N 4 synthesized from trithiocyanuric acid (TCA-CN) showed the largest SSA (56.59 m 2 /g), the narrowest band gap (2.621 eV), and lowest carriers’ recombination rate, which correspondingly exhibited the best photocatalytic performance for the degradation of bisphenol A (BPA). Moreover, the g-C 3 N 4 synthesized by urea (U-CN) demonstrating the strongest photoelectron density, widest band gap (2.790 eV) and the most positive VB potential showed the highest activating efficiencies of all three oxidants. In general, persulfates were more competent to enhance the degradation of BPA than H 2 O 2 , and PMS showed the highest activity. The dominant reactive oxidation species (ROS) depended more on the type of peroxides than on the catalyst precursors. The effective activation of PDS by U-CN was primarily resulting from the photoelectrons to produce extra •OH to enhance compounds degradation, and high yield of 1 O 2 could be achieved by PMS activation through h + oxidation, leading to the most significant enhancement of BPA removal. The N–C 3 and NH x of U-CN were likely the sites for PMS activation. Moreover, the U-CN/LED/PMS process showed the strong adaptability to the complex water environment. This work may provide new insights into selecting highly efficient g-C 3 N 4 -based advanced oxidation processes for water remediation.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2023
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IF 9.9
Qun Ding,Xuejun Zou,Jun Ke,Yuying Dong,Yubo Cui,Hongchao Ma
Herein, a ternary TiO 2 /MIL-88A(Fe)/g-C 3 N 4 heterojunction is successfully constructed through a facile hydrothermal strategy for enhancing solar energy harvesting and efficiency of catalytic nitrogen reduction induced by enlarged light absorption range, increasing interfacial charge transfer ability and desirable stability. Under the simulated sunlight irradiation, the N 2 fixation experiment shows that the yield of NH 3 reaches 1084.31 μmol/(g·h) over the TiO 2 /MIL-88A(Fe)/g-C 3 N 4 photocatalyst, and the yield is significantly enhanced, which is 33.68 and 13.94 times that is higher than the pure TiO 2 and g-C 3 N 4 , respectively. In a mean time, the excellent performance of the photocatalytic N 2 fixation over the ternary TiO 2 /MIL-88A(Fe)/g-C 3 N 4 is verified based on density function theory calculation and the decisive step over the composite is investigated by calculating Gibbs free energies of nitrogen reduction paths. The performance enhancement mechanism of TiO 2 /MIL-88A(Fe)/g-C 3 N 4 is speculated, which indicates that the hybridized three-component system presents a desirable Z-scheme band alignment, resulting in the improvement of separation and transfer efficiency of photoinduced charge carriers. The article shows a new and high-efficiency TiO 2 /MIL-88A(Fe)/g-C 3 N 4 photocatalysis for excellent nitrogen reduction ability.
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International Journal of Electrochemical Science
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2023
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IF 1.5
Jun Chen,Boding Zhang,Bingxing Wang,Chengxing Cui,Songlin Wang,Jichao Wang,Wenlong Zhang
With high toxicity, carcinogenicity and teratogenicity, quinoline has been threatening human health and ecological environment. Herein, Fe-Co-Ni-P/g-C 3 N 4 particles are developed as electrochemical reactors to form a three-dimensional catalytic particle electrode system (3D-CPE) for efficient removal of quinoline from wastewater by electro-Fenton (EF) oxidation process. with reaction time of 30 min, the particles dosage of 50 g/L, pH of 3, conductivity of 11.5 ms/cm, and current density of 37.04 mA/cm 2 , the chemical oxygen demand (COD) removal rate can up to 90.95%. In addition, electron paramagnetic response (EPR) and radical scavenging tests are performed to determine the hydroxyl radicals of electrochemical processes produced. The degradation products are analyzed by high performance liquid chromatography-mass spectrometry (HPLC-MS). Finally, through theoretical calculation and analysis of degradation products, a reasonable degradation mechanism is proposed.
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RSC Advances
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2023
·Vol. 13
·期 22
·15302-15310
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IF 3.9
Deng Gu,Yuanjin Wang,Zhiman Liang,Yanting Dou,Zhenhe Xu,Jiqi Zheng,Yaguang Sun,Fu Ding,Yu Gao
The construction of a heterojunction and the introduction of a cocatalyst can both promote the transfer of photogenerated electrons, which are effective strategies to enhance photocatalytic efficiency. In this paper, a ternary RGO/g-C3N4/LaCO3OH composite was synthesized by constructing a g-C3N4/LaCO3OH heterojunction and introducing a non-noble metal cocatalyst RGO through hydrothermal reactions. TEM, XRD, XPS, UV-vis diffuse reflectance spectroscopy, photo-electrochemistry and PL tests were carried out to characterize the structures, morphologies and carrier separation efficiencies of products. Benefiting from the boosted visible light absorption capability, reduced charge transfer resistance and facilitated photogenerated carrier separation, the visible light photocatalytic activity of the ternary RGO/g-C3N4/LaCO3OH composite was effectively improved, resulting in a much increased MO (methyl orange) degradation rate of 0.0326 min−1 compared with LaCO3OH (0.0003 min−1) and g-C3N4 (0.0083 min−1). Moreover, by combining the results of the active species trapping experiment with the bandgap structure of each component, the mechanism of the MO photodegradation process was proposed.
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