Surfaces and Interfaces
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2024
·
IF 5.7
Leizhi Zheng,Yang Xu,Chenyang Huang,Jia Liu,Lei Zhou,Chengbao Liu
Graphitic carbon nitride (g-C 3 N 4 ) containing conjugated tri-s-triazine units has a high abundance of amine and guanidine groups, which are ideal for the application of CO 2 conversion. However, absolute g-C 3 N 4 is inherently scarce in Lewis base sites, which leads to low catalytic activities. In this study, we present a simple and green method to in situ construct chrysanthemum stalk-derived porous carbon/ highly active defective g-C 3 N 4 (PC/g-C 3 N 4 ) through hydrogen bond, increasing the surface area and a high density of Lewis base sites. The chrysanthemum stalk contains cellulose, hemicellulose and lignin, which possess a significant number of hydroxyl functional groups and drain channels, thereby providing more hydrogen bonding for highly active defective g-C 3 N 4 . The XPS spectra revealed that, in comparison to PC/g-C 3 N 4 –1 and PC/ g-C 3 N 4 –2.5, PC/g-C 3 N 4 –2 exhibited a higher C-NH 2 content at the edge of the nitrogen element. PC/g-C 3 N 4 –2 had a high specific surface area to expose more active sites for absorbing CO 2 . The quantification of the base sites is determined by the peak area of the thermal programmed desorption of CO 2 and is 229.6 μmol/g for PC/g-C 3 N 4 –2. PC/g-C 3 N 4 –2 demonstrated excellent catalytic activity in the cycloaddition with hierarchical pores. The yield of cyclic carbonate was up to 99% with a selectivity of 99% under mild solvent-free conditions. The mechanistic studies indicate that PC/g-C 3 N 4 –2 not only captured CO 2 , but also provided hydrogen bonds to activate the oxygen atom of epichlorohydrin (ECH). It is our contention that the multifunctional organic-inorganic hybrid materials have considerable potential for the production of cyclic carbonate.
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Nanomaterials
·
2024
·
IF 4.4
Fangqin Liu,Mingjie Fan,Xia Liu,Jinyang Chen
A cellulose-based carbon aerogel (CTN) loaded with titanium dioxide (TiO 2 ) and graphitic carbon nitride (g-C 3 N 4 ) was prepared using sol–gel, freeze-drying, and high-temperature carbonization methods. The formation of the sol–gel was carried out through a one-pot method using refining papermaking pulp, tetrabutyl titanate, and urea as raw materials and hectorite as a cross-linking and reinforcing agent. Due to the cross-linking ability of hectorite, the carbonized aerogel maintained a porous structure and had a large specific surface area with low density (0.0209 g/cm 3 ). The analysis of XRD, XPS, and Raman spectra revealed that the titanium dioxide (TiO 2 ) and graphitic carbon nitride (g-C 3 N 4 ) were uniformly distributed in the CTN, while TEM and SEM observations demonstrated the uniformly distributed three-dimensional porous structure of CTN. The photocatalytic activity of the CTN was determined according to its ability to degrade rhodamine B. The removal rate reached 89% under visible light after 120 min. In addition, the CTN was still stable after five reuse cycles. The proposed catalyst exhibits excellent photocatalytic performance under visible light conditions.
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CHEMICAL ENGINEERING JOURNAL
·
2025
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IF 13.2
Dandan Wang,Jing Li,Rong Zhang,Beiyu Xin,Xueru Huang,Yang Wang,Jifeng Guo
Microcystis aeruginosa (M. aeruginosa) is a typical harmful algal associated with eutrophication, making the study of its inactivation critical for water restoration. In this research, g-C 3 N 4 /CeO 2 composites with S-scheme heterojunctions were synthesized and incorporated into sodium alginate (SA) to successfully prepare photocatalytic gel beads with floating capabilities. A photocatalytic persulfate (g-C 3 N 4 /CeO 2 /SA/Vis/PMS) system was developed to systematically investigate the algal inactivation efficacy of floating catalysts. The g-C 3 N 4 /CeO 2 S-scheme heterojunctions significantly enhanced algal inactivation efficiency, achieving up to 96.65 % inactivation within 80 min. The alterations in algal cell properties during the inactivation process were examined. A decrease in the content of algal bile proteins indicated a disruption of the photosynthetic system within the algal cells, while an increase in the concentrations of K + , Ca 2+ , and Mg 2+ suggested further disruption of algal cell membranes and walls. Additionally, three-dimensional fluorescence spectroscopy (EEM) results indicated that the extracellular organic matter produced during the rupture of algal cells was degraded into humic acid-like substances. The energy bands and electronic structure of g-C 3 N 4 /CeO 2 were calculated using density functional theory (DFT) to analyze the electron transfer mechanism involved in this process, which is consistent with the S-scheme electron transfer pathway. The effective inactivation of M. aeruginosa was successfully achieved through the combined action of the non-radical 1 O 2 ,·O 2 – , and h + generated during the photogenerated carrier transfer process. This approach offers a promising strategy for the management of algal blooms in eutrophic waters.
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Journal of Water Process Engineering
·
2025
·
IF 6.7
Yang Yu,Lichao Xu,Kaiyuan Xu,Yan Li,Hao Chen,Dongxu Zhang,Yuanzi Chen,Yue Liu,Wenyue Qi
The construction of S-scheme heterojunctions has drawn widespread attention within the photocatalysis field due to their capacity for efficient separation of photogenerated carriers, leading to excellent photo-oxidation-reduction performance. Herein, a novel S-scheme loofah biochar/MoS 2 /g-C 3 N 4 (LB/MS/CN) heterojunction was successfully constructed by ultrasonication in 50 % ethyl alcohol and heat treatment in N 2 atmosphere. Degradation experiments showed that the 5 % LB/MS/CN ternary photocatalyst had optimal photocatalytic efficiency (96.4 %) for the degradation of rhodamine B (RhB), and the reaction rate (k) of this photocatalyst (0.05420 min −1 ) was 5.4 times that of unmodified CN (0.01001 min −1 ). Ultraviolet-visible diffuse reflectance spectra, Mott-Schottky, and free radical trapping experiments suggested that the photogenerated carriers in LB/MS/CN were transferred through the S-scheme structure. Consequently, the co-catalytic action of LB and the synergistic impact of the heterojunction structure between CN and MS led to a reduced photogenerated carrier recombination rate. Furthermore, LB/MS/CN had outstanding stability and the capacity to maintain RhB degradation performance under various environmental conditions (H 2 PO 4 − , NO 3 − , SO 4 2− , HCO 3 − , NaCl, humic acid (HA), and real water), showing good promise for practical applications. Thus, this work provides a possible strategy for purifying wastewater under visible light.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2018
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IF 11.698
Longbo Jiang,Xingzhong Yuan,Guangming Zeng,Jie Liang,Xiaohong Chen,Hanbo Yu,Hou Wang,Zhibin Wu,Jin Zhang,Ting Xiong
Artificial Z-scheme photocatalyst can not only reduce the recombination of photogeneraged electron–holepairs, but also retain prominent redox ability. In this study, direct solid-state dual Z-scheme WO 3 /g-C 3 N 4 /Bi 2 O 3 photocatalyst was successfully synthesized by one step co-calcination stratage using tungstic acid, melamine and bismuth (III) nitrate pentahydrate as the precursors. Surface, morphological, and structural properties of the resulting materials were comprehensive characterized by XRD, XPS, SEM, TEM, UV–vis diffuse reflection spectroscopy, BET surface areas, photoluminescence and ESR analysis. The WO 3 /g-C 3 N 4 /Bi 2 O 3 composite exhibited superior photocatalytic activities for tetracycline degradation than that of pure g-C 3 N 4 , WO 3 , Bi 2 O 3 and their binary composites under visible light irradiation. The enhanced photocatalytic performance of WO 3 /g-C 3 N 4 /Bi 2 O 3 composite can be ascribed to improved visible light absorption, increased surface area and enhanced separation efficiency of photo-generated electron-hole pairs. In addition, the photocatalyst exhibits high stability and reusability. On the basis of the results, a novel direct solid-state dual Z-scheme photocatalytic mechanism was also proposed.
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NEW JOURNAL OF CHEMISTRY
·
2017
·Vol. 42
·期 3
·1771-1778
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IF 3.269
Saisai Cheng,Xufeng Meng,Ningzhao Shang,Shutao Gao,Cheng Feng,Chun Wang,Zhi Wang
Well-dispersed Pd nanoparticles were anchored on g-C3N4 nanosheets, which were prepared by a liquid-phase exfoliation method. The hybrid material displayed excellent catalytic activity for the transfer hydrogenation of nitroarenes. The reactions can be conducted smoothly in water at room temperature with formic acid as hydrogen source. Aniline was produced in excellent yield (>99%; turnover frequency: 853), surpassing the majority of reported heterogeneous catalysts using formic acid or formates as hydrogen source. The increased activity of such a hybrid catalyst can be ascribed to the nitrogen-rich and amphipathic property of the carbon nitride support, the stable and uniform dispersed Pd nanoparticles and the Mott–Schottky effect between the g-C3N4 nanosheets and the metal nanoparticles. The heterogeneous Mott–Schottky catalyst can be reused for five cycles without any obvious loss of its catalytic activity.
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DALTON TRANSACTIONS
·
2017
·Vol. 47
·期 4
·1284-1293
·
IF 4.029
Yingfei Wang,Fengliang Wang,Yiping Feng,Zhijie Xie,Qianxin Zhang,Xiaoyu Jin,Haijin Liu,Yang Liu,Wenying Lv,Guoguang Liu
The development of facile and efficient synthetic approaches of carbon quantum dots loaded with mesoporous g-C3N4 (mpg-C3N4/CQDs) is of critical urgency. Here, a facile strategy was developed to synthesize the mpg-C3N4/CQDs by using calcinations of the mixture of CQDs, cyanamide, and silica colloid. The obtained composite still retained a considerable total surface area, which could offer a larger population of adsorption sites; therefore enhance the capacity for the adsorption of fluoroquinolones antibiotics (FQs). Under visible light irradiation, mpg-C3N4/CQDs demonstrated a higher photocatalytic activity for FQs degradation than did bulk g-C3N4 or mpg-C3N4. This enhancement might have been ascribed to the high surface area of the mpg-C3N4, unique up-converted photoluminescence (PL) properties, and the efficient charge separation of the CQDs. The eradication of FQs followed the Langmuir–Hinshelwood (L–H) kinetic degradation model and absorption pseudo-second-order kinetic model, indicating that surface reactions and chemical sorption played significant roles during the photocatalysis process. The results of electron spin resonance (ESR) technology and reactive species (RSs) scavenging experiments revealed that the superoxide anion radical (O2˙−) and photo-hole (h+) were the primarily active species that initiated the degradation of FQs. Based on the identification of intermediates and the prediction of reactive sites, the degradation pathways of ofloxacin (OFX) were proposed. A residual antibiotic activity experiment revealed that mpg-C3N4/CQDs provided very desirable performance for the reduction of antibiotic activity.
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CATALYSIS LETTERS
·
2024
·
IF 2.3
Ren Zongli,Zhao Zhongwei,Ma Xin,Zhang Weiwei
Construction of multi-interface contact step-scheme (S-scheme) photocatalyst is a promising pathway to achieve high-electron transfer efficiency for photodegradation estrone and congo red. In this paper, g-C 3 N 4 is chosen as the main photocatalyst, CeO 2 nanosheet with the unique Ce 4+ → Ce 3+ conversion performance and Fe 3 O 4 -Reduced graphene oxide are loaded onto the g-C 3 N 4 surface to bulid 2D-2D magnetic photocatalyst. The 2D–2D magnetic photocatalyst structure imparts reusability by magnetic retrieval and at the same time Fe 3 O 4 -Reduced graphene oxide acts as an efficient host for g-C 3 N 4 /CeO 2 composite photocatalyst. The photocatalytic performance is examined using etsrone and congo red. Photodegradation studies show the CeO 2 /g-C 3 N 4 / Fe 3 O 4 - Reduced graphene oxide a composite catalyst can degrade 71% of estrone, 92% of congo red and 89% phenanthrene, Free radical scavenger test shows superoxide and hydroxyl radical species play a major role in the degradation. Furthermore, it is demonstrated that the magnetic CeO 2 /g-C 3 N 4 / Fe 3 O 4 -Reduced graphene oxide possesses strong antibacterial properties against Proteus mirabilis and Escherichia coli. A three-factor-three-level Box–Behnken design (BBD) was selected to optimize three greatly influential parameters: light irradiation time (min), The quality of photocatalyst(mg) and pollution concentration(ppm) by response surface methodology. It is expected that CeO 2 /g-C 3 N 4 / Fe 3 O 4 - Reduced graphene oxide can be used as a 2D–2D magnetic photocatalyst for to achieve its valorization, which have very broad development prospects in the field of environmental remediation or catalysis. Graphical Abstract
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Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Qingtong Cao,Bing Wang,Guomin Li,Xinzhong Wang,Jian Zhang,Hongxin Lv
Due to the high biological toxicity and the propensity to induce antibiotic resistance, the treatment of antibiotic wastewater has consistently posed a formidable challenge. The semiconductor photocatalysts can efficiently and completely remove antibiotics from the wastewater to repair the water environment. Therefore, a novel ZnIn 2 S 4 /Tb-g-C 3 N 4 (ZIS/TCN) photocatalyst was successfully synthesized in this paper and its ability to efficiently degrade antibiotics has been verified. The optimized 150ZIS/TCN photocatalyst showed excellent photocatalytic performance and stablility toward the degradation of tetracycline (TC) and tylosin (TYL) under sunlight simulated with a xenon lamp. Compared with pristine g-C 3 N 4 and ZnIn 2 S 4 , the 150ZIS/TCN exhibited superior degradation performance for TC (TYL)，about 3.2 (2.1) and 1.8 (1.5) times higher than them. Based on density functional theory (DFT) calculations and experimental characterization test results, it was confirmed that the Tb doping effectively regulates the intrinsic electric field and visible light absorption capacity. This study unveils the degradation mechanism of ZIS/TCN photocatalysis and provides an effective pathway for enhancing photocatalytic degradation through rare earth doping.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2024
·
IF 4.9
Jingjing Xu,Jingyi Wei,Yanying Cui,Sixian Yu,Sufang Guo,Qi An,Ping Han
In this work, an Au/g-C 3 N 4 /GO/Au hybrid nanofilm for surface-enhanced Raman scattering (SERS) substrate application was prepared by a facile layer-by-layer assembly technique using nanosheet-structured graphitic carbon nitride (g-C 3 N 4 ), graphene oxide (GO) and 40 nm-gold nanoparticles (Au NPs). The effects of composition, assembly sequence and assembly cycles on the SERS performance were optimized to achieve the SERS-active substrate. The detection limit of Au/g-C 3 N 4 /GO/Au substrate for crystal violet and rhodamine 6 G probe molecules reached as high as 10 -8 M, with good stability and uniformity. Its further application in food colorants detection (erythrosine, carmine and temptation red) had successfully met the national food safety standards and the quantitative detection for erythrosine and temptation red had also been established. Based on finite-difference time-domain element simulation and density functional theory quantum chemical calculation, the mechanism of the SERS effect of the substrate was unveiled, which is attributed to the combination of electromagnetic enhancement effect of Au nanoparticle aggregates and chemical enhancement effect of GO and g-C 3 N 4 . Notably, water droplet evaporation induced Raman enhancement was observed on the Au/g-C 3 N 4 /GO/Au substrate. This can be ascribed to the inhomogeneous evaporation of the droplet that promotes the enrichment of the probe molecules into the center of the droplet. This novel enhancement strategy provides a new idea for further improving detection sensitivity of SERS substrate materials.
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Advanced Powder Materials
·
2024
·
IF 28.6
Lei Li,Xinyan Dai,Meichi Lu,Changfa Guo,Saikh Mohammad Wabaidur,Xi-Lin Wu,Zhangrong Lou,Yijun Zhong,Yong Hu
Modulating electronic structures of single-atom metal cocatalysts is vital for highly active photoreduction of CO 2 , and it's especially challenging to develop a facile method to modify the dispersion of atomical photocatalytic sites. We herein report an ion-loading pyrolysis route to in-situ anchor Pd single atoms as well as twinned Pd nanoparticles on ultra-thin graphitic carbon nitride nanosheets (Pd TP /Pd SA -CN) for high-efficiency photoreduction of CO 2 . The anchored Pd twinned nanoparticles donate electrons to adjacent single Pd–N 4 sites through the carbon nitride networks, and the optimized Pd TP /Pd SA -CN photocatalyst exhibits a CO evolution rate up to 46.5 μmol g −1 h −1 with nearly 100% selectivity. As revealed by spectroscopic and theoretical analyses, the superior photocatalytic activity is attributed to the lowered desorption barrier of carbonyl species at electron-enriched Pd single atoms, together with the improved efficiencies of light-harvesting and charge separation/transport. This work has demonstrated the engineering of the electron density of single active sites with twinned metal nanoparticles assisted by strong electronic interaction with the support of the atomic metal, and unveiled the underlying mechanism for expedited photocatalytic efficiency.
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CHINESE JOURNAL OF CATALYSIS
·
2025
·
IF 17.7
Yang Zhang,Nengneng Xu,Bingbing Gong,Xiaoxiao Ye,Yi Yang,Zhaodi Wang,Biyan Zhuang,Min Wang,Woochul Yang,Guicheng Liu,Joong Kee Lee,Jinli Qiao
Storing solar energy in battery systems is crucial to achieving a green and sustainable society. However, the efficient development of photo-enhanced zinc-air batteries (ZABs) is limited by the rapid recombination of photogenerated carriers on the photocathode. In this work, the visible-light-driven CoS 2 /CuS@CNT-C 3 N 4 photocatalyst with unique petal-like layer structure was designed and developed, which can be used as air electrode for visible-light-driven ZABs. The superior performance of ZABs assembled by CoS 2 /CuS@CNT-C 3 N 4 was mainly attributed to the successful construction of Schottky heterojunction between g-C 3 N 4 and carbon nanotubes (CNTs), which accelerates the transfer of electrons from g-C 3 N 4 to CoS 2 /CuS cocatalysts, improves the carrier separation ability, and extends the carrier lifetime. Thereinto, the visible-driven ZABs assembled by CoS 2 /CuS@CNT-C 3 N 4 photocatalyst has a power density of 588.90 mW cm –2 and a charge-discharge cycle of 643 h under visible light irradiation, which is the highest performance ever reported for photo-enhanced ZABs. More importantly, the charge-discharge voltage drop of ZABs was only 0.54 V under visible light irradiation, which is significantly lower than the voltage drop (0.94 V) in the dark. This study provides a new idea for designing efficient and stable visible-light-driven ZABs cathode catalysts.
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