INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2024
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IF 8.1
Yijun Luo,Zhendong Liu,Jincheng Liu,Wei Cai,Zewei Liao,Xuyang Feng,Jia Zheng,Chengzhi Zhang,Yanxiong Fang
The photocatalytic efficiency of graphitic carbon nitride (g-C 3 N 4 ) in hydrogen production is primarily hindered by its poor absorption of visible light , rapid recombination of electron-hole pairs, and the absence of hydroxyl radical formation. Herein, a novel g-C 3 N 4 nanosheets functionalized with sulfonic acid groups were effectively produced through thermal polymerization of melamine and 2, 4-diamino-6-phenyl-1, 3, 5-triazine (DPT), followed by sulfonation treatment. The introduction of the phenyl group brings about alterations to the initial symmetrical arrangement of g-C 3 N 4 , leading to the disruption of certain hydrogen bonds . This, in turn, facilitates the movement of electrons from the n to π* orbitals, resulting in enhanced light absorption and improved efficiency in charge separation. Moreover, it induces modifications to the band structure and amplifies the production of hydroxyl radicals. Additionally, the introduction of sulfonic acid enhances the water affinity and the ability of dispersing graphitic carbon nitride in water. The optimized sulfonated benzene-substituted g-C 3 N 4 (1000-BCN-SO 3 H) with a melamine to DPT ratio of 4:1 exhibits a maximum hydrogen production rate of 6.52 mmol·h −1 ·g −1 under simulated sunlight irradiation with good cycling stability, which is 3.93 times higher than that of g-C 3 N 4 nanosheets . This research offers a promising opportunity for a novel approach in advancing carbon nitride materials for effective photocatalytic processes.
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MATERIALS SCIENCE IN SEMICONDUCTOR PROCESSING
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2024
·
IF 4.2
Min Yuan,Ke Huang,Dongqing Dai,Hongfei Yin,Wei Zhao,Yixin Jiang,Yahui Feng
The integration of heterogeneous photocatalysts has emerged as a promising approach to boost the effectiveness of photocatalytic reactions for hydrogen evolution. In this study, we explore the synergistic effects of Ti 3+ -TiO 2 /P-doped g-C 3 N 4 heterojunctions on the enhancement of visible light-induced hydrogen generation efficiency. The photocatalytic hydrogen evolution performance of the as-prepared TPCN100 (280.38 μmol g −1 h −1 ) surpasses that of pristine P-doped g-C 3 N 4 (34.89 μmol g −1 h −1 ) and Ti 3+ -TiO 2 (39.71 μmol g −1 h −1 ) by factors of 8.0 and 7.1 respectively. Through a comprehensive investigation of the structural, electronic, and photocatalytic properties, the underlying mechanisms accountable for the observed enhancement in efficiency within the heterojunction system were elucidated. Based on the in-situ X-ray photoelectron spectrometer (XPS) examination, measurement of band edge, and electron paramagnetic resonance (EPR) analysis, the S-scheme photocatalytic mechanism was proposed. The integration of Ti 3+ -TiO 2 and P-doped g-C 3 N 4 offers new insights into the design of advanced photocatalytic materials for sustainable energy applications.
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INORGANIC CHEMISTRY
·
2024
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IF 4.3
Xiaorong Gan,Leilei Ye,Huimin Zhao,Dangyuan Lei,Yanhui Ao,Dan Zhao,Peifang Wang
Microenvironments in heterogeneous catalysis have been recognized as equally important as the types and amounts of active sites for regulating catalytic activity. Two-dimensional (2D) nanospaces between van der Waals (vdW) gaps of layered materials provide an ideal microenvironment to create novel functionalities. Here, we explore a facile method for fabricating g-C3N4/2H-MoS2 superlattice-like heterostructures based on thermochemical intercalation and polymerization reactions of formamide within enlarged vdW gaps of 2H-MoS2 nanosheets without any transfer process. DFT calculations demonstrate that the interlayer electron–electron correlations due to the intercalation effect of g-C3N4, rather than high-κ dielectric environments, lead to the improvement of intrinsic conductivity of 2H-MoS2 nanosheets. As the proof of concept in applications for the electrocatalysis field, the heterostructure for hydrogen electrochemical reaction (HER) exhibits high stability and catalytic activity in both acid and alkaline media, such as a quite low onset overpotential of 98 mV, a high exchange current density of 77.6 μA cm–2, and a small Tafel slope (52.9 mV dec–1) in an acid medium. The enhanced HER activity is attributed to the improved conductivity and nanoconfinement effect of 2D nanospaces that decrease the reaction activation energy and activate the inert basal planes.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
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IF 8.1
Yangyang Dai,Tian Fang,Shumin Li,Yuanyuan Wang,Suyue Zhong,Wenjun Su,Jian Li
While mixed matrix membranes (MMMs) containing two-dimensional (2D) layered materials (such as, GO, g-C 3 N 4 and MXene , etc.) have revealed potential application prospects for gas separation applications, it still faces a serious challenge to enhance the performance of CO 2 separation. Owing to the structural defects of g-C 3 N 4 nanosheets produced during the exfoliation process, which has greatly reduced the gas selectivity. Herein, we describe the construction of g-C 3 N 4 -MXene/Pebax MMM composed by MXene modified the structural defects in g-C 3 N 4 nanosheets to surmount the low gas selectivity of g-C 3 N 4 membrane. However, the stacking of nanosheets on each other hinder the gas transport channels. The TiO 2 nanoparticles derived in-situ from MXene semi-oxidation can support an intermediate layer between g-C 3 N 4 nanosheet and MXene nanosheet to expand the gas transport channels. Eventually, a novel g-C 3 N 4 -TiO 2 @MXene/Pebax MMM was obtained that exhibited maximum CO 2 permeability of 1673.69 Barrer in separation of CO 2 /CH 4 , CO 2 /N 2 selectivity of 45.13, and CO 2 /CH 4 selectivity of 47.76, exceeding the bond 2008 limit on Robeson. What's more, the MMM within 100 h (1 bar and 298 K) are measured to have outstanding separation performance. Overall, this concept offers a novel strategy to enhance CO 2 separation by MXene modified defects in g-C 3 N 4 nanosheets.
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ChemSusChem
·
2024
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IF 7.5
Dong Li,Kaixuan Wang,Ying Chen,Renyi Li,Jiahong Tang,Yizhou Zhao,Wei Guo,Qi Chen,Yujing Li
Graphical A 0D/1D CPB@TCN heterojunction photocatalyst for CO 2 reduction is synthesized by immobilizing CsPbBr 3 (CPB) quantum dots on one-dimensional porous tubular g-C 3 N 4 (TCN). The strong Pb−N chemical bonding between CPB quantum dots and TCN provides a fast charge transfer channel for the CPB@TCN, which promotes the efficient separation and transfer of photogenerated carriers, resulting in excellent photocatalytic activity. Halide perovskite CsPbBr 3 (CPB) quantum dots (QDs) are considered as a promising candidate for solar-driven CO 2 conversion for their unique optoelectronic properties and suitable band structures. However, the CO 2 conversion efficiency of pristine CsPbBr 3 quantum dots is severely limited due to their rapid electron-hole pair recombination and insufficient active sites. In this study, by immobilizing CPB QDs onto one-dimensional (1D) porous tubular g-C 3 N 4 (TCN), an effective 0D/1D CPB@TCN heterojunction photocatalyst for CO 2 reduction is fabricated. Density functional theory (DFT) calculations combined with experimental studies demonstrate that CPB QDs are uniformly anchored on the surface of TCN through Pb−N chemical bonding, resulting in efficient separation and transfer of photogenerated carriers in CPB@TCN photocatalysts. The resultant CPB@TCN photocatalysts exhibit significantly enhanced photocatalytic activity for CO 2 reduction with the highest conversion rate of 22.62 μmol g −1 h −1 , which is 5.33-times higher than that of pristine CPB QDs. This work unveils the interfacial bonding mechanism of CPB@TCN heterojunction through Pb−N chemical bond, which provides new insights for the development perovskite-based heterojunction photocatalysts.
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CHEMICAL ENGINEERING JOURNAL
·
2024
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IF 13.3
Guanhan Chen,Wenhui Ding,Wenyi Dong,Hongjie Wang,Shuting Zhu,Tianzhe Liang,Cheng Luo,Yuxiong Huang
The wide occurrence of pharmaceutically active contaminants (PhACs) in aquatic environments has received more and more concern owing to the associated high risks to ecosystems. Even worse, conventional wastewater treatment techniques fail to provide effective decontamination for these emerging contaminants . Herein, we designed and constructed mAg 3 PO 4 @g-C 3 N 4 heterojunction for a persulfate-assisted photocatalytic system (mAg 3 PO 4 @g-C 3 N 4 /PDS/Vis) for the rapid and effective degradation of PhACs. Superior mineralization of CBZ (87.15 %) was achieved within 30-minute treatment with mAg 3 PO 4 @g-C 3 N 4 /PDS/Vis, exhibiting 11-fold enhancement compared to mAg 3 PO 4 /Vis system. Integrating experimental investigations with theoretical calculations, singlet oxygen ( 1 O 2 ) was identified as the key reactive species, while the 1 O 2 -dominated ring-opening pathway contributed significantly to the high mineralization of CBZ. Moreover, mAg 3 PO 4 @g-C 3 N 4 /PDS/Vis showed robust degradation performance of multiple PhACs across various water matrices. Multiple PhACs could be simultaneously degraded with high mineralization efficiency in the wastewater effluent, demonstrating the promising application of mAg 3 PO 4 @g-C 3 N 4 /PDS/Vis for decontaminating emerging contaminants in wastewater treatment .
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DIAMOND AND RELATED MATERIALS
·
2024
·
IF 4.3
Jingle Zhang,Huihu Wang,Yangliu Ou,Hao Tu,Ziguan Zhang,Chenhuinan Wei,Xing Xiang,Ming Bao
As the overuse of antibiotics increasingly contaminates the environment, one of modern chemistry's objectives is to identify high-performance photocatalytic materials to degrade antibiotics. This study initially utilized NH 4 Cl as a gas template to synthesize porous lamellar g-C 3 N 4 (CNS) through a high-temperature calcination process. Building upon this, a homojunction catalyst, CNS/g-C 3 N 5 (S-CN), was developed via a secondary sintering technique using different amount of 3-amino-1,2,4-triazole addition to evaluate its efficacy in activating peroxymonosulfate (PMS) for degrading the antibiotic ceftriaxone sodium. Under neutral conditions, the photocatalytic system composed of S-CN catalysts prepared by 50 mg of 3-amino-1,2,4-triazole addition and PMS (S 3 -CN/PMS) exhibited degradation rates that were 3.37 and 8.11 times higher than those of the CNS/PMS and g-C 3 N 5 /PMS, respectively. At a pH of 8, the S 3 -CN/PMS system attained a 99.7 % degradation efficiency within 75 min. Based on results from UV–visible diffuse reflectance spectroscopy (DRS), transient photocurrent response, electrochemical impedance spectroscopy (EIS), photoluminescence spectroscopy and radical scavenging experiments, this high efficiency is attributed to a homojunction Z-type charge transfer mechanism that enhances the separation of photogenerated carriers. Furthermore, the study found that the optimal PMS addition was 20 mg and the optimal pH was 8. Chloride ions promoted the reaction, while other ions decreased the reaction rate. In conclusion, this paper provides valuable insights for the morphological modification of carbon nitride homojunction materials and the efficient activation of PMS for pollutant degradation.
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CERAMICS INTERNATIONAL
·
2024
·
IF 5.1
Yunqi Ning,Daqi Lv,Qi Tang,Hanbing Wang,Xiaowan Hu,Yuming Cao,Shansheng Yu,Hongwei Tian
Photocatalysts for hydrogen evolution reaction (HER) have widely been explored but fine-tuning and engineering multiphase photocatalyst components are still challenging. Among catalysts, ZnIn 2 S 4 has shown promise but maximizing the use of ZnIn 2 S 4 -photogenerated carriers and enhancing quantum yield still require further investigation. One way to achieve this is by enhancing the photon utilization and reducing the recombination of shallow carriers in ZnIn 2 S 4 . Accordingly, novel ZnIn 2 S 4 /g-C 3 N 4 /MoS 2 type-II heterojunction composites with 2D/2D/2D structures (abbreviated ZIS/CN/MS) were synthesized in the present work by simple thermal condensation-solvothermal method. The optimized ZIS/CN/MS exhibited a photocatalytic hydrogen evolution rate of 13.6 mmol g −1 h −1 under visible light (λ ≥ 420 nm) irradiation, a value much higher than those of pure-phases ZIS and CN, as well as the binary composite of ZIS/CN. The apparent quantum efficiency of the optimized ZIS/CN/MS at a wavelength of 420 nm reached 27.0 % coupled with excellent cycling stability. The significantly improved photocatalytic performance and the excellent stability can mainly be attributed to the unique 2D/2D/2D arrangement of the ternary components of ZIS, CN, and MS in ZIS/CN/MS photocatalyst, providing a large number of close interfacial contacts between the components for shortened migration distance of photogenerated charges and more pathways for electron separation and transport in type-II heterostructures. Overall, the proposed methodology and ZIS/CN/MS composites with type-II heterojunction and 2D/2D/2D structures have great potential for use in solar-to-hydrogen energy conversion and can be extended to the preparation of other photocatalysts.
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MATERIALS CHEMISTRY AND PHYSICS
·
2024
·
IF 4.3
Shizheng Zhang,Hongliang Xu,Qianqian Qin,Chaoning Huang,Yongqiang Niu,Mingliang Li,Bo Song,Bingbing Fan,Gang Shao,Hongxia Lu,Hailong Wang
Vermiculite/g-C 3 N 4 /BiOBr composite (MCVB-X, X = 20, 50, 70, 90) with significantly improved photocatalytic performance was prepared by in-situ growing 20 wt%, 50 wt%, 70 wt%, 90 wt% of BiOBr nanosheets , respectively, on the surface of vermiculite/g-C 3 N 4 composite (MVC). With the increasing of BiOBr content, the photocatalytic performance of MCVB-X composites enhanced gradually. After 180 min of photocatalytic reaction under the visible light irradiation , the degradation rate of tetracycline (TC) by MCVB-50, which contained 50 wt% of BiOBr, reached 91.34 %, which was close to that of pure BiOBr and much higher than those of MVC and bulk g-C 3 N 4 (CN). The reaction rate constant (k) (0.0131 min −1 ) of MVCB-90 was 38.53 times and 6.24 times that of CN and MVC, respectively, which was also greater than that of pure BiOBr nanosheets (0.0098 min −1 ). The main reason for the significant improvement of photocatalytic performance of MCVB-X composites was that the construction of g-C 3 N 4 /BiOBr heterojunction promoted the separation and migration of photogenerated carriers and reduced the recombination rate of photogenerated electron-hole pairs. The agglomeration of BiOBr nanosheets was inhibited and contributed to the adsorption of pollutants. Moreover, the band structure , main active species (⋅O 2 − ) and photocatalytic degradation mechanism were proposed.
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RSC Advances
·
2025
·Vol. 15
·期 2
·1311-1322
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IF 4.6
Wenzhe Li,Xudong Wang,Ye Chen,Pengcheng Wu,Zhengtao Li,Zhiqiang Wang,Deng Gu
Loading with non-metal cocatalysts to regulate interfacial charge transfer and separation has become a prominent focus in current research. In this study, g-C3N4/CNT composites loaded with non-metallic cocatalysts were prepared through in situ pyrolysis using urea and CNTs. Various characterization techniques, including transmission electron microscopy (TEM), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), ultraviolet-visible diffuse reflectance spectroscopy (UV-vis DRS), photoelectrochemical (PEC) analysis, fluorescence lifetime spectroscopy (TRPL), electron paramagnetic resonance spectroscopy (ESR), and photoluminescence (PL) spectroscopy, were employed to analyze the sample's microstructure, phase composition, elemental chemical states, and photoelectronic properties. The photocatalytic performance of the g-C3N4/CNT composite in the degradation of actual drilling hydraulic filtrate was evaluated under simulated sunlight irradiation, with the degradation results assessed through COD and chroma measurements. The findings indicate that in g-C3N4/CNT composites loaded with non-metal cocatalysts, the photocatalytic performance improves significantly as the CNT content increases. At a CNT mass fraction of 6.0%, the composite achieves optimal performance, with a COD degradation rate of 0.3742 h−1 and a chroma degradation rate of 81%. These results offer valuable insights into enhancing photocatalytic treatment of waste drilling hydraulic filtrate using g-C3N4-based non-metallic cocatalysts.
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Science China-Materials
·
2024
·Vol. 67
·期 7
·2142-2152
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IF 6.8
Li Yaying,Yang Huijuan,Li Jili,Li Yefei,Ren Wei,Wen Jin,Xiao Qi,Xu Jingsan
Heterojunction photocatalysis has been widely studied as a means of efficiently converting solar energy to chemicals. However, the major challenge in developing high-performing heterojunction photocatalytic systems lies in achieving efficient transfer of electrons between the components. Herein, a novel S-scheme heterojunction photocatalyst was developed by combining BaTi 2 O5 nanorods with g-C 3 N 4 lamellae. The preferential deposition of Pt nanoparticles as cocatalyst via the one-step impregnation-reduction method on g-C 3 N 4 nanosheets with enhanced interfacial contact and strong electronic interaction has been proved essential for the photocatalytic performance. The developed Pti mp /20BaTi 2 O 5 /g-C 3 N 4 photocatalyst delivers the optimal hydrogen production rate of 2587 µmol g −1 h −1 with high stability after cycles. Photoelectrochemical analysis and theoretical calculation suggest that the formation of BaTi 2 O 5 /g-C 3 N 4 heterojunction results in the staggered band alignment and improved charge carrier dynamics. This work highlights the importance and feasibility of promoting photocatalysis by a new S-scheme heterojunction with viable cocatalysts.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2024
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IF 4.9
Lingyi Zhang,Jiachun Wu,Hongyun Xu,Huixia Li,Xiang Liu,Yanhua Song,Yanjuan Cui
The fabrication of non-metallic semiconductor heterojunction with superior redox capability for hydrogen (H 2 ) evolution from water and environmental remediation has been emerging as a prospective strategy. Herein, a novel two-dimensional (2D) g-C 3 N 4 /Ni-MOF Z-scheme heterojunction was prepared by a facile sonication-gel self-assembly method with g-C 3 N 4 and nickel metal-organic framework (Ni-MOF) nanosheets . The ultra-thin nanosheet structure of Ni-MOF was conducive to the formation of stable 2D heterojunctions. The opposite surface charge and matched band difference caused the charge flow from g-C 3 N 4 to Ni-MOF, resulting in an interfacial built-in electric field. The optimized NMF/CN-9 attained the optimal 3aphotocatalytic activity towards the degradation of tetracycline (TC) and H 2 evolution from water. Under visible light irradiation , the reaction rate for TC degradation (0.00497 min −1 ) and H 2 evolution (15.6 μmol·h −1 ) over NMF/CN-9 was nearly 2.4 and 2.1 folds higher than that of g-C 3 N 4 , respectively. Besides, the photocatalytic performance of NMF/CN-9 was also nearly 2 times higher than that of g-C 3 N 4 under simulated solar illumination. Such improvements were originated from higher photo-excited charge separation and superior redox ability derived from Z-scheme interfacial charge transfer. A possible photocatalytic mechanism was also proposed and the results indicated that efficient photo-induced electrons and reactive hole (h + ), superoxide radical (·O 2 - ) and hydroxyl radical (·OH) played a major role during the photocatalytic route. This work offers an intense insight into the construction of non-metallic semiconductor 2D heterojunctions for H 2 evolution and environmental wastewater treatment .
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