JOURNAL OF ALLOYS AND COMPOUNDS
·
2026
·
IF 6.3
WU Xiaocui,Kan Chen,Wenxiu Xue,Fenghao Sun,Huiying Yang,Zhaojie Cui
Organic dye pollutants have posed a significant threat to aquatic ecosystems. Graphitic carbon nitride (g-C 3 N 4 ), as a metal-free photocatalyst with broad application potential, has been widely explored for the degradation of environmental pollutants. However, its practical efficiency is severely limited by a low specific surface area and a high recombination rate of photogenerated electron-hole pairs. Furthermore, its performance is highly sensitive to synthesis parameters such as method, temperature, and precursor ratio. To address this, this study developed a multilayer perceptron-artificial neural network (MLP-ANN) model to quantify parameter impacts on Rhodamine B (RhB) degradation rate, integrating four synthesis methods (template-free, soft/hard/self-template), material characterization, and mechanistic analysis. MLP-ANN (R 2 =0.9774, outperforming random forest R 2 =0.563) identified melamine (FI=0.33), urea (FI=0.19), and silica template (FI=0.11) as key factors (for porous structure) and catalyst concentration (FI=0.17, increasing active sites) as dominant in reactions. Guided by the model, self-template g-C 3 N 4 (g-C 3 N 4 -SeT) showed optimal performance: k= 0.0613 min −1 , ∼100 % RhB degradation (43.8 times better than template-free g-C 3 N 4 -TF). SEM/TEM confirmed uniform porosity in g-C 3 N 4 -SeT, while UV-Vis DRS and PL showed the enhanced visible-light absorption and suppressed carrier recombination. Superoxide radicals (•O 2 - ) were proved as the main active species. Efficient separation of electron-hole pairs by g-C 3 N 4 -SeT promotes the generation of •O 2 - , thereby accelerating RhB degradation. This work demonstrates the successful integration of machine learning with experimental characterization to optimize both the synthesis strategy and photocatalytic performance of g-C 3 N 4 , establishing a data-driven framework for the rational design of advanced functional catalysts.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Chenghong Wu,Xiaopeng Chen,Jiezhen Liang,Jiawei Fu,Zhongyao Zhang,Xiaojie Wei,Linlin Wang
The catalytic hydrogenation of dicyclopentadiene (DCPD) is one of the pivotal processes in the production of green high-energy-density liquid hydrocarbon fuels, jet propellent-10 (JP-10). However, the high dependency of the current catalysts on high temperature and pressure, whether the non-noble (>120 ℃, >15 bar) or even the noble catalyst (80 ℃, >7.6 bar), leads to enormous energy consumption and technical challenges in environment and sustainable development. Herein, we prepared a carbon layer wrapped Ni nanoparticles/g-C 3 N 4 catalyst (Ni@C/g-C 3 N 4 ) derived from the in-situ-formed Ni-MOF/g-C 3 N 4 composite. Benefiting from the 53.2 wt% small-sized Ni nanoparticles and nanosheet structure, resulting in high-density accessible active sites (5.38 × 10 20 sites g −1 ) and the mass transfer enhancement, Ni@C/g-C 3 N 4 achieved DCPD hydrogenation under ambient conditions. > 99.9 % DCPD conversion and 98.1 % endo -tetrahydrodicyclopentadiene yield was obtained at 30 ℃, 1 bar, significantly outperforming the benchmark 5 % Pd/C. To the best of our knowledge, it’s the mildest condition for DCPD hydrogenation. Further, comprehensive mechanistic insights were gained from combining means of kinetic investigations, in situ characterization, and theoretical calculations. The discrimination result of 27 kinetic models indicated that DCPD hydrogenation followed the Langmuir-Hinshelwood-Haugen-Watson formulism regarding the reaction between the chemisorbed dihydrodicyclopentadiene (DHDCPD) and dissociatively adsorbed hydrogen as the rate-determining step. In-situ DRIFTS confirm that the norbornene ring is preferentially adsorbed and hydrogenated. The DFT calculations further substantiate the hydrogenation pathway. The present work provides guidance for the development of highly efficient non-noble metal catalysts and opens up an environmental-friendly and economically viable avenue for DCPD hydrogenation.
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Biochar
·
2023
·Vol. 5
·期 1
·1-20
·
IF 12.7
Yang Bowen,Dai Jiawei,Zhao Yuan,Wang Zhanchao,Wu Jingwei,Ji Caiya,Zhang Yuhu,Pu Xiao
Biochar-coupled Fe 3 O 4 @SiO 2 /TiO 2 /g-C 3 N 4 composites were successfully constructed through simple sol–gel and calcination methods. The composites efficiently removed high-concentration toxic tetracycline (TC) by means of ·OH and · \({\rm O}_2^{-}\) , whose removal rate exhibited 91.88% during 3 h, and the degradation rate constant reached up to 0.0068 min −1 . The excellent performance can be attributed to the high specific surface area, enhanced visible light response, the introduction of magnetic nanoparticles and biochars expediting charge transfer, Z-scheme heterojunction enhancing the spatial separation of photo-generate carriers and, importantly extraordinary adsorption capacity of 147.96 mg g −1 . Moreover, the composites showed the most excellent efficiency under the calcination temperature of 450 ℃, and exhibited good stability with tolerance to a wide range of pH and anions. Interestingly, a synergistic photocatalytic effect was discovered in the TC/Cr(VI) combined pollution systems, resulting in significantly improved removal of Cr(VI). Besides, the photocatalytic mechanism and degradation path of tetracycline were also elucidated. All these findings suggested the as-synthesized catalyst was an excellent photocatalyst for removal of TC/Cr(VI)-contaminated water. Graphical Abstract
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Materials Today Communications
·
2022
·
IF 3.662
Junyue Shan,Xianliang Wu,Caifang Li,Jiwei Hu,Zhenming Zhang,Huijuan Liu,Pinhua Xia,Xianfei Huang
In recent years, semiconductor materials have shown excellent potential in the field of photocatalytic degradation of antibiotics. To prepare a photocatalyst with excellent performance, an Fe 3 O 4 /rGO/Co-doped ZnO/g-C 3 N 4 tetrameric hybrid photocatalyst was successfully prepared for the first time by means of chemical precipitation using graphene oxide as the precursor. The developed quaternary photocatalyst was used for the degradation of oxytetracycline hydrochloride (OTC), and its photocatalytic activity was investigated. The structure and morphology of the composites were characterized by XRD , SEM, HR-TEM, ESR, N 2 adsorption, PL spectroscopy and UV-Vis DRS . The effects of different parameters on the degradation process were studied by the response surface method and artificial intelligence. The results showed that Fe 3 O 4 /rGO/Co-doped ZnO/g-C 3 N 4 was successfully synthesized. Under optimal conditions, the degradation rate of OTC was approximately 82% (the Fe 3 O 4 /rGO/Co-doped ZnO/g-C 3 N 4 dose was 0.16 g, the pH was 7.0, the initial concentration of OTC was 30 mg/L, and the visible light irradiation time was 70 min). pH is the most influential variable for OTC removal. At the same time, the degradation rate of OTC remained above 50% after 5 times of recycling, indicating that Fe 3 O 4 /rGO/Co-doped ZnO/g-C 3 N 4 photocatalyst had good stability and recoverability. In addition, the results of ESR and radical trapping experiments showed that·O 2 - and·OH were the main active species in the OTC removal process.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2022
·
IF 6.371
Jian Wang,Changchun Chen,Zhihao Zhao,Cheng Cheng,Zhonghai Tang,Zhou Du,Yifeng Wang,Lin Pan
Considerable attentions are currently paid to water pollution, which seriously threats human health. Semiconductor catalysts with step-like (S-scheme) heterojunction are often used for degrading organic pollutants in water bodies due to their high carrier separation efficiency, high redox capacity, and broad light absorption capacity. In this paper, a novel S-scheme N-doped g-C 3 N 4 /NH 2 -MIL-125(Ti) heterojunction composite is synthesized for photodegradation of organic pollutants. The structural measurements indicate that the NH 2 -MIL-125(Ti) nanoparticles are intimately anchored on the surface of porous N-doped g-C 3 N 4 nanosheets . The experimental characterizations as well as the DFT theoretical calculation for samples demonstrate that the N-doped g-C 3 N 4 /NH 2 -MIL-125(Ti) composites not only bear larger specific surface area providing abundant reactive sites, but also improve the separation efficiency of photogenerated carriers during photodegradation. In addition, the degradation rate of RhB solution catalyzed by 25 wt% N-doped g-C 3 N 4 /NH 2 -MIL-125(Ti) (25 wt% NCM) attains the highest degradation rate (96.4%) under visible light irradiation. Moreover, the mineralization of RhB solution and intermediates produced in the degradation process are analyzed by total organic carbon (TOC) and high- performance liquid chromatography (HPLC) tests, respectively. Electron paramagnetic resonance (EPR) with free radical capture measurements show that the photodegradation of RhB is mainly ascribed to the superoxide radicals (·O 2 - ) and hole (h + ). This study provides an effective method to construct S-scheme heterojunction photocatalysts and apply them to wastewater treatment.
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SCIENCE OF THE TOTAL ENVIRONMENT
·
2022
·
IF 10.753
Tongtong Wang,Jiyong Zheng,Jinjun Cai,Qiangqiang Liu,Xianxia Zhang
To improve the performance of graphitic carbon nitride (g-C 3 N 4 ), a hotly researched metal-free photocatalyst, for better application in the efficient removal of organic pollutants, adsorption synergistically enhanced photocatalysis mechanism was thoroughly explored. Based on KOH pore-forming activated biochar (ACB) and K + doped g-C 3 N 4 (K-gC 3 N 4 ), the novel activated biochar-based K-gC 3 N 4 composite (ACB-K-gC 3 N 4 ) was synthesized via the innovative ultrasonic-milling method. Rhodamine B (RhB), tetracycline (TC), norfloxacin (NOR), and chloramphenicol (CAP) were selected as target pollutants, and the effects of environmental factors, recycling and actual wastewater tests, disinfection effects, and various enhancement strategies were investigated. The results showed that K-gC 3 N 4 was successfully composited with ACB by various characterizations, where the loading mass ratio of 1:2 exhibited the best performance. ACB-K-gC 3 N 4 possessed a larger specific surface area, richer functional groups, suitable band gap (2.29 eV), and broader visible light absorption (~716 nm) than K-gC 3 N 4 . ACB-K-gC 3 N 4 presented effective removal efficiency over K-gC 3 N 4 for four pollutants, in which the removal efficiency of RhB reached 93.26%, and the degradation rate constant of 0.0119 min −1 was four times higher than K-gC 3 N 4 (0.0029 min −1 ). Moreover, ACB-K-gC 3 N 4 was superior to K-gC 3 N 4 in disinfecting S. aureus and E. coli , with a sterilization rate of exceeding 90% for 12 h. The photodegradation activity was dominated by · O 2 − , h + , and · OH, and the mechanisms involved in the three stages. This was attributed to the unique structure and surface properties (defects and persistent free radicals) of ACB, as evidenced by improved adsorption stage and transfer of degradation intermediates, facilitated the generation of active species, accelerated migration of photogenerated electrons, and inhibited photogenerated carriers recombination by the heterojunction . The good reusability and stability, enhancement strategies (blowing air and heating), and satisfactory feasibility for actual wastewater allow ACB-K-gC 3 N 4 possible to promote high-concentration wastewater treatment and disinfection.
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NEW JOURNAL OF CHEMISTRY
·
2022
·Vol. 46
·期 14
·6738-6746
·
IF 3.925
Xin Dai,Xian-Yi Jin,Rui-Han Gao,Qing-Mei Ge,Kai Chen,Nan Jiang,Hang Cong,Zhu Tao,Mao Liu
Photoelectrochemical water splitting based on g-C3N4 is considered as a promising approach to oxygen generation. Hereinto, an innovative photoanode, g-C3N4/Q[6]–Co NPs, is successfully fabricated by depositing a Co nanocatalyst on the surface of a g-C3N4 film. The nanoparticles are prepared by reduction of a coordination compound of Co[II]–cucurbit[6]uril, in which the macrocycle served as a template and supporter. The resulting g-C3N4/Q[6]–Co NPs provided a significant improvement of the photocurrent density (393 μA cm−2 at 1.23 V vs. RHE) and a higher photoconversion efficiency (0.02419%) than the pristine g-C3N4 catalyst. These results reveal that the high visible light absorption of g-C3N4/Q[6]–Co NPs ensures the formation of a large number of photogenerated electron–hole pairs, and therefore the holes are immediately transferred to the g-C3N4 film through the semiconductor–metal interface, inhibiting the charge recombination process and increasing the photocurrent performance. The approach proposed in this study not only provides a new strategy, in which a macrocyclic compound is employed as the template and supporter in the synthetic process of the nanocatalyst, but also opens a new window for the application of g-C3N4 in PEC water splitting.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2022
·
IF 5.518
Yongkun Lun,Shuting Hu,Fuming Chen,Qinyu He,Yinzhen Wang,Wei Li,Guannan He
In this work, an S-scheme heterojunction-structured composite, g-C 3 N 4 /Mo-doped WO 3 (mass ratio 100:5, labeled 5M15WOCN) together with pure WO 3 , g-C 3 N 4 , and Mo-doped WO 3 (labeled M15WO) was prepared. The as-prepared samples were characterized by XRD , UV–Vis DRS, SEM, TEM, ESR , EIS , PL and XPS . The photocatalytic properties were investigated by photodegrading methyl orange (MO). The following findings were obtained. The dopant Mo increased the amount of O v -s and produced W 5+ , along with prolonging the lifetime of photogenerated carriers, improving the transfer ability of carriers. The S-scheme heterojunction g-C 3 N 4 /M15WO drastically improved the photocatalytic properties, dominantly due to the synergetic effect of the O v -s, S-scheme mechanism and very negative CB potential. A new phenomenon is found in which W 6+ can combine with the net electrons coming from the side with a higher Fermi level in the heterojunction and form W 5+ , suggesting a good method for stabilizing the high valence state for the material by combining one with a lower Fermi level. This work also implies that, compared to the S-scheme, a more negative CB is much more beneficial for MO photodegradation .
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JOURNAL OF SOLID STATE ELECTROCHEMISTRY
·
2022
·Vol. 26
·期 4
·959-971
·
IF 2.747
Lin Yu,Wu Yeyu,Tan Xuecai,Wu Jiawen,Huang Kejing,Mi Yan,Ou Panpan,Wei Fucun
An ultrasensitive “signal-off–on” electrochemiluminescence (ECL) biosensor is constructed based on f1-TiO 2 /g-C 3 N 4 /PDA for thrombin detection. The flower-like titanium dioxide (f1-TiO 2 ) has a huge specific surface area, which can not only increase the capacity of 2D graphite-like carbon nitride (g-C 3 N 4 ) layer, but also promote the action of coreactants, and the ECL intensity of the electrode modified with f1-TiO 2 /g-C 3 N 4 /PDA is 3.5 times higher than the electrode modified with g-C 3 N 4 /PDA. The carboxylated thrombin aptamer (sDNA) is incubated onto the modified electrode by amide bond; then, the complementary strand of thrombin aptamer (tDNA) modified with ferrocene is connected to the electrode surface by complementary base pairing with sDNA. Due to the ferrocene can quench the ECL of g-C 3 N 4 , the ECL signal decreases, while the ECL signal is restored in the presence of the target thrombin (TB). When K 2 S 2 O 8 and H 2 O 2 are used as a co-reactant, the ECL aptasensor for TB detection is constructed with a concentration variation from 10 −11 to 10 −5 M, which has a excellent sensitivity, and the detection limit is 8.9 × 10 −12 M. It also shows good specificity, reproducibility, and stability. This novel ECL aptasensor has potential application in human thrombin assay.
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Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Yu Wang,Yuxin He,Yujing Chi,Peiji Yin,Lishan Wei,Wenwen Liu,Xinyao Wang,Han Zhang,Haiyan Song
Photocatalytic H 2 O 2 production is a green and sustainable technology, which still exposes the issues of excessive dependence on organic electron donors and pure O 2 , and lacking effective use. It is necessary to develop more efficient and more economical photocatalysis system for H 2 O 2 production. Here, we construct a S-scheme p-n heterojunction from the p-type MnS and the n-type protonated g-C 3 N 4 (PCN) semiconductors for photocatalytic H 2 O 2 production and achieve the in situ use of H 2 O 2 for oxidative degradation of oxytetracycline (OTC). The PCN/MnS composite synthesized by a one-step method well maintains a nanosphere structure of α-MnS and load the PCN on the sphere surface to form a heterojunction with strong interaction. PCN/MnS exhibits the improved photogenerated charge separation and electron transfer efficiency. An optimal photocatalyst can produce 669.6 μM of H 2 O 2 for 6 h without using the electron donors and the pure O 2 gas. The mechanism proposed the contribution of a S-scheme p-n heterojunction forms between PCN and MnS. The electrons in conduction band (CB) of MnS are responsible for the major single-electron reduction of •O 2 - radicals and the auxiliary two-electron reduction of O 2 for H 2 O 2 production, while the holes in valence band (VB) of PCN further promote the separation of photocarriers. The photogenerated H 2 O 2 can be effectively used as an in-situ oxidant to achieve 82.2% degradation of OTC in water within 80 min. The •O 2 - radicals which originate from the in situ decomposition of H 2 O 2 over PCN/MnS mainly contribute to the OTC oxidation .
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2021
·
IF 5.816
Yuan Ding,Zhi Lin,Jiawei Deng,Yingliang Liu,Li Zhang,Kunlun Wang,Shengang Xu,Shaokui Cao
In this work, a series of carbon dots (CDs) modified hollow g-C 3 N 4 spheres (HCNS-C x ) were constructed via a double in situ approach using cyanamide and glucose as precursors, respectively. As HCNS-C x was synthesized by one-step in situ thermal polymerization of two precursors, which could make CDs and g-C 3 N 4 keep tight connection and increase the separation of the photogenerated electron-hole pairs. The average diameter and wall thickness of the HCNS-C x are about 355 nm and 55 nm, respectively. Under the visible light irradiation , the H 2 evolution rate (HER) of HCNS-C 1.0 (2322 μmol g −1 h −1 ) was 19 times that of bulk g-C 3 N 4 (122 μmol g −1 h −1 ) and 1.8 times that of HCNS without CDs modification (1289 μmol g −1 h −1 ), respectively. And its apparent quantum efficiency is 17.93% at 420 nm. The specific surface area, light absorption capacity , and charge carrier mobility of HCNS-C x could be dramatically improved due to the introduction of CDs and hollow structures of g-C 3 N 4 spheres, resulting in a significant improvement of photocatalytic activity .
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JOURNAL OF HAZARDOUS MATERIALS
·
2021
·
IF 10.588
Mengmeng Dou,Jin Wang,Zhaokun Ma,Boru Gao,Xue Huang
In the study, an efficient ‘1 + 1 > 2′ synergistic coupling system driven by visible light consisting of mesoporous g-C 3 N 4 (MCN) and persulfate (PS)was constructed. The free radical transformation, electron transfer and non-covalent interaction between the MCN layer and PS in the system were explored via experiments and DFT calculations. The similarity for the fate of the seven β-lactam antibiotics with typical structures in the oxidation system was studied systematically in depth. First, the consistencies and differences of the seven antibiotics were summarized from three aspects: three-dimensional structures, electron cloud distributions, and the vulnerable sites. Notably, the selective differential degradation of β-lactam antibiotics in the MCN/PS system was speculated to be related with the molecular ionization potential (MIP), as a key index to describe the difficulty of oxidation. The distribution relationship between MIP and the oxidation kinetic constant ( K ) was explored and showed the following trend: a higher MIP indicates a weaker ability to provide electrons, and this leads to a greater resistance to oxidative degradation. In total, four main oxidation pathways of β-lactam antibiotics were systematically summarized combining HPLC-QTOF-MS and the simplified Fukui function calculation. The toxicity assessment of intermediate products provided by the T.E.S.T software of USEPA also shows a decreasing trend in the oxidation process. In the end, the superior practicability and stability of the MCN/PS system was verified by complex environment simulation and cyclic test. This research clarified the selective differential degradation mechanism of β-lactam antibiotics and provided a possible idea for the effective removal of refractory organic pollutants in water.
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