ChemCatChem
·
2025
·
IF 3.9
Tianao Zhang,Haolong Huang,Yunchong Wang,Qianqian Zhao,Rui Han,Qingling Liu
Graphical CoO x /BCN catalyst with dual active sites was successfully synthesized. This catalyst exhibits excellent selectivity (99%) and a cyclic carbonate yield (98%) in the CO 2 cycloaddition reaction with the nucleophilic reagent KI under solvent-free and mild reaction conditions. This catalyst also has good stability and reusability, providing a new direction for the design of high-performance CO 2 cycloaddition catalysts. The carbon dioxide (CO 2 ) cycloaddition reaction provides an efficient route to achieve resource utilization of CO 2 . However, the inherent chemical stability of CO 2 itself hinders its efficient transformation into cyclic carbonates. Herein, the CoO x /BCN catalyst was successfully prepared by a simple deposition method. The CoO x /BCN exhibited excellent catalytic performance in the CO 2 cycloaddition reaction synergistically catalyzed with the nucleophilic reagent KI under solvent-free and mild reaction conditions (80 °C, 0.8 MPa, 6 h). The yield of cyclic carbonate was 98% and the selectivity was 99%, which was significantly superior to CoO x /CN catalyst (with a cyclic carbonate yield of 73.7%). Furthermore, after six cyclic reactions, CoO x /BCN still maintained a yield of over 93%. It was found that after boron (B) was doped into graphitic carbon nitride (g-C 3 N 4 ), the generated ─NB(OH) 2 group on CoO x /BCN effectively activated the epoxide. Importantly, the interaction between B-doped g-C 3 N 4 and CoO x induced the generation of abundant oxygen vacancies, which provided sufficient active sites for CO 2 adsorption and activation. In addition, carbonates were identified as the main reaction intermediates by in situ DRIFTS, and the possible reaction pathways of the CoO x /BCN catalyst were proposed. Therefore, this work provides new idea for the design of catalysts for CO 2 cycloaddition.
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高影响因子
APPLIED ORGANOMETALLIC CHEMISTRY
·
2025
·Vol. 39
·期 9
·e70348
·
IF 0
Yongguang Wang,Yi Pei,Siqi Hu,Chunxin Lu,Wei Zhong,Zhiyin Xiao,Junjie Wang,Xiaoming Liu
In this work, the preparation and characterization of a composite of Cu-Cu 2 O with g-C 3 N 4 and its application in the catalysis of aerobic oxidation of benzylic alcohols are reported. The composites Cu-Cu 2 O/g-C 3 N 4 were prepared starting with CuSO 4 under reduction conditions with ball milling, followed by thermal treatment. The introduction of g-C 3 N 4 into the composite can enhance the catalytic oxidation. Band structure analysis based on UPS data reveals that the enhancement can be attributed to the small work function of g-C 3 N 4 , which raises the VBM level of the chief catalyst Cu 2 O through injecting electrons into the oxide at the heterojunction due to Fermi energy alignment. Both VBM ascending and forming an internal electric field (IEF) due to the electron transfer across the interface contribute to the enhancement in the catalysis. Further, the N-rich matrix g-C 3 N 4 promotes proton transfer in the catalysis due to its basicity, which also accelerates the catalysis.
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ADVANCED FUNCTIONAL MATERIALS
·
2021
·Vol. 32
·期 15
·2111125
·
IF 18.808
Binyao Liu,Jinyan Du,Gaili Ke,Bi Jia,Yujie Huang,Huichao He,Yong Zhou,Zhigang Zou
g -C 3 N 4 photocatalysis is a safe and green approach for H 2 O 2 production, but the activity of pristine g -C 3 N 4 photocatalysts is unsatisfactory. At present, most of the modifications on g -C 3 N 4 photocatalysts for H 2 O 2 production have focused on thermodynamic processes, few have considered the kinetic aspects. Herein, the surface N -hydroxymethylation of g -C 3 N 4 photocatalysts for the efficient kinetic production of H 2 O 2 is reported. Through the reaction of formaldehyde with the amino moieties (–NH 2 ) on the g -C 3 N 4 surface, N -hydroxymethyls groups (-NH-CH 2 -OH) are introduced on typical g -C 3 N 4 photocatalysts. Relative to the pristine g -C 3 N 4 photocatalysts, the modified g -C 3 N 4 photocatalysts have over 1280% higher activity for H 2 O 2 production in pure water system, and impressive solar-to-chemical conversion efficiency. The experimental investigations and theoretical calculations reveal that the introduction of -NH-CH 2 -OH on the g -C 3 N 4 photocatalysts does not change their morphology, light absorption intensity and edges, band positions, charge separation and transfer properties, but markedly improved the H 2 O dehydrogenation and O 2 adsorption properties of g -C 3 N 4 . As a result, the reduction kinetics of O 2 to H 2 O 2 on the g -C 3 N 4 photocatalysts with -NH-CH 2 -OH is more energetically favorable. This work provides a useful reference and inspiration to achieve the effective modification of g -C 3 N 4 or other metal-free photocatalysts from the kinetic perspective.
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高影响因子
ENVIRONMENTAL RESEARCH
·
2025
·
IF 7.7
Yehan Xiong,Tiantian Xu,Bingchang Chen,Jiangkun Du,Lijing Tan,Yujie Zhong,Jianguo Bao
The photocatalytic performance of materials is primarily governed by their band structure, charge carrier transport, and active sites. This study introduces a surface modification strategy for graphitic carbon nitride (g-C 3 N 4 ) using C=O groups to significantly enhance its photocatalytic activity. The C=O-modified g-C 3 N 4 (CNSHQC2) demonstrated exceptional photocatalytic performance. It achieved a degradation rate of over 85 % for tetracycline hydrochloride (TC) in five different real wastewater matrices within 40 min of natural sunlight exposure. By combining quantitative structure-activity relationship analysis with site-specific blocking experiments, the C=O groups were identified as the primary active sites. Traditional functional group modifications typically improve photocatalytic performance by increasing surface area or enhancing charge transfer. In contrast, C=O modification simultaneously optimizes the band structure and introduces active sites that promote PMS activation. The results indicate that this dual modulation of electronic structure and surface chemistry facilitates efficient charge carrier separation and enhances the generation of reactive oxygen species (ROS). Additionally, C=O groups increase triplet exciton generation and promote singlet oxygen formation via energy transfer. These synergistic effects collectively contribute to a significant improvement in the photocatalytic performance of g-C 3 N 4 . This work provides a new strategy for designing high-performance photocatalysts and valuable insights into the role of C=O groups in expanding the potential applications of carbon-based materials in environmental remediation.
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PubMed
高影响因子
ACS Applied Engineering Materials
·
2025
·
IF 3.5
Feng Lin,He Liu,Yu Tang,Xuejun Zheng,Hui Dong
Two-dimensional (2D) materials are widely used in heavy metal ion detection due to their high specific surface area and abundant active sites. Herein, we prepared highly selective and sensitive electrochemical sensors based on 2D graphitic-phase carbon nitride for the detection of Cu2+ and Pb2+ ions and investigated the effects of both tensile and compressive strains on the corresponding detection sensitivity, together with their mechanism. The prepared carbon nitride nanosheet sensors showed detection sensitivities of 3.63 and 0.41 μA·μM·cm–2, detection ranges of 0.2–100 and 6–100 μM, and detection limits of 0.0033 and 0.23 μM for Cu2+ and Pb2+, respectively. The induced compressive strain of −0.25% in the 2D CNNS significantly improved the sensitivity by 40.5% and 31.7%, while the tensile strain of +0.25% reduced the sensitivity by 41.9% and 43.9% in detecting Cu2+ and Pb2+ as compared to those at zero strain, respectively. Through DFT calculations, the corresponding compressive strain of −0.25% reduced the band gap from 1.21 eV under zero strain to 0.94 eV. On the contrary, the tensile strain of +0.25% increased the band gap from 1.21 to 1.45 eV, resulting from the contribution of orbitals of C-p and N-p. The declined and raised band gaps, respectively, result in increased and decreased electron transport rates, thereby improving and degrading the sensitivities of the sensors. Our research provides guidance on the design of flexible wearable sensors integrated into the construction of sensitive and reliable heavy ion detection systems.
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高影响因子
COMPOSITES COMMUNICATIONS
·
2025
·
IF 7.7
Wei Wang,Hong Cao,Jian You,Yongzhao Li,Weihe Yu,Huaiyin Chen,Longmin Liu,Meihua Wu,Yuekun Lai,Weilong Cai
As the raw material for fabricating polyphenylene sulfide (PPS) fibers, PPS resin exhibits great processing and application value. However, the oxidative cross-linking among PPS molecules at high temperatures causes increasing melt viscosity and decreasing fluidity, making PPS processing difficult and lower production quality and efficiency. In this research, we realize the dual improvement of PPS resin in the fluidity and oxidation resistance by introducing a new AO-g-C 3 N 4 composite modifier. First, an antioxidant (AO) was grafted onto the surface of graphitic carbon nitride (g-C 3 N 4 ) through amination to synthesize AO-g-C 3 N 4 . Subsequently, AO-g-C 3 N 4 was incorporated into PPS resin using the melt extrusion process, yielding a novel flow-enhancing and antioxidant PPS-based composite material. It is found that the AO-g-C 3 N 4 /PPS material possesses excellent properties with a significantly raised melt index (>50 %) and notably decreased shear viscosity (>20 %). Besides, the dynamic oxidation induction temperature of AO-g-C 3 N 4 /PPS has increased, indicating inhibited oxidative cross-linking, while the crystallinity has increased. These suggest that the incorporation of AO-g-C 3 N 4 into PPS resin can enhance its fluidity and antioxidation properties, providing valuable insight for the modification research of PPS resin. The AO-g-C 3 N 4 /PPS exhibits the characteristic of easier processing, which offers promising prospects for developing the downstream industry of PPS resin.
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高影响因子
MATERIALS RESEARCH BULLETIN
·
2025
·
IF 5.7
Yan Wang,Hui Liu,Wenzhi Li,Na Li,Guoyong Wang,Xiaochao Zhang
Rational structural design of S-scheme heterojunctions in semiconductor-based photocatalysts constituted a pivotal strategy for optimizing their photocatalytic performance through efficient charge carriers separation and enhanced redox capability. Herein, a novel two-dimensional 2D/2D heterostructure is successfully constructed by integrating bismuth oxychloride (BiOCl) nanosheets onto g-C 3 N 4 nanosheets, which significantly enhances the interfacial contact area between these two components and facilitates the migration of photogenerated charge carriers by forming a built-in electric field. Specifically, thiourea, urea, and melamine are employed as the precursor to prepare a series of g-C 3 N 4 /BiOCl photocatalysts, denoted as T-CN/BiOCl, U-CN/BiOCl, and M-CN/BiOCl, respectively. Benefiting from the excellent hydrophilic characteristics, wide photoresponse ranges and efficient interfacial charge transfer, M-CN/BiOCl displays exceptional degradation performance for both cationic rhodamine B (RhB) dyes and anionic methyl orange (MO). Under simulated sunlight irradiation, the photocatalytic degradation of RhB (20 mg/L) and MO (20 mg/L) can exhibit distinct kinetics, with complete removal achieves in 10 min and 100 min , respectively. Notably, the degradation rate constants of RhB demonstrate the remarkable superiority, being 29.2-fold and 475.2-fold higher than those of MO under simulated sunlight and visible light irradiation.
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高影响因子
Journal of Zhejiang University-SCIENCE A
·
2025
·
IF 3.9
Li Xianhua,Yu Qingbo
To explore high value-added utilization pathways of fly ash, the mesoporous structure of silicon dioxide extracted from fly ash (FA-SiO 2 ) was utilized to restrict the dicyandiamide (DCDA) thermal degradation process. This produced chemically bonded interacting composite photocatalysts of FA-SiO 2 and graphitic-phase carbon nitride (g-C 3 N 4 ). Compared with the spherical silicon dioxide prepared using tetraethyl orthosilicate (TEOS-SiO 2 ), the mesoporous structure of FA-SiO 2 allowed DCDA to react in a smaller space, which facilitated the transformation of DCDA to melamine by the thermal degradation kinetics of FA-SiO 2 /DCDA. This ultimately boosted the formation of an N-atom-removed triazine ring structure and a multistage structure combining lumps and rods in the composite photocatalysts of g-C 3 N 4 and FA-SiO 2 , which led to a higher visible-light utilization efficiency, a suitable valence-band position, and the photocatalytic activity for methylene blue reaching 3.56 times that of g-C 3 N 4 . The findings indicate that mesoporous FA-SiO 2 has the potential to improve the structural and photocatalytic properties of g-C 3 N 4 -based materials.
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Yao Huang,Xuefeng Hu,Chuanyi Wang,Detlef Bahnemann
Donor-acceptor (D-A) structure has gained momentous attention due to its controllable optical band gap and impressive carrier separation performance. The intramolecular charge transfer within photocatalysts could be modulated by constructing a D-A structure, thereby enhancing their performance in degrading pollutants. In our recent research, using poly(3-bromothiophene) (PTh-Br) and dicyandiamide (DCD) as precursors, a series of D-A structures (CN-PTh-Br(x)) based on polythiophene donors and carbon nitride acceptors were obtained by one-pot synthesis for first-time. The density functional theory calculations further demonstrate that PTh-Br segment (an electron donor) donates electrons to tri-s-triazine rings (an electron acceptor). The introduction of electron-rich polythiophene groups and electron-withdrawing Br atoms on carbon nitride skeleton can propel the transfer and separation of holes and electrons. Moreover, the polythiophene groups with high conjugation length can optimize the optical absorption of CN-PTh-Br(x) at 450–600 nm, thus markedly heightening the visible-light utilization efficiency of the materials. The photocatalytic performance of CN-PTh-Br(x) was assessed through the photodegradation of 2-mercaptobenzothiazole (MBT) under visible-light illumination. The photodegradation performance of CN-PTh-Br(0.5) stood out among all the samples, demonstrating a remarkable ability to remove 99.8% of MBT within 45 min.
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高影响因子
FUEL
·
2025
·
IF 7.5
Shiyu Wang,Shuai Wang,Mingmei Ge,Yang Zhao,Hua Song,Huan Wang
This work introduces a template-free strategy for preparing three-dimensional (3D) honeycomb-like graphitic carbon nitride (g-C 3 N 4 ) with high specific surface area through phosphoric acid-regulated supramolecular self-assembly. By systematically tuning phosphoric acid dosage, the self-assembly process of melamine-cyanuric acid aggregates is precisely controlled, resulting in a hierarchically porous architecture with interconnected channels and abundant porosity. The optimized phosphoric acid-mediated support (SSCN-0.89) enables uniform dispersion and stabilization of ultrafine Pt nanoparticles (∼1.7 nm) via enhanced metal-support interactions. Under mild conditions (120 ℃, 0.5 MPa H 2 ), the resultant Pt/SSCN-0.89 catalyst achieves 94.1 % phenol conversion within 80 min with exclusive cyclohexanol selectivity (100 %). Mechanistic studies reveal that the hierarchical porous structure facilitates rapid mass transfer, while the tailored surface nitrogen species lower the reaction energy barrier. The catalyst retains robust stability over five cycles, demonstrating the pivotal role of 3D morphological engineering in designing high-performance carbon nitride-based catalytic supports for biomass upgrading.
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高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Wentao Liu,Qiu Wang,Zhi Liu,Guixiang Ding
A series of treble NiAl-LDH/g-C 3 N 4 /carbon quantum dots (LDH/CN/CQDs) photocatalysts is successfully prepared for the photoreduction of CO 2 to CO via a facile hydrothermal pathway. In the 3D flower-like LDH/CN/CQDs, CQDs not only achieve the efficient inhibition of charge recombination but also act as the unhindered “electronic bridges” to synergistically construct a classical type-Ⅱ charge transfer configuration, which synchronously permits the effluence of photogenerated electrons from CN to LDH and holes from LDH to CN, and promotes ultraviolet–visible irradiation respondence. The sample of LDH/CN/CQDs-6 is the optimal one amongst the LDH/CN/CQDs with a larger special surface area (98.43 m 2 g −1 ) and an appropriate content of CQDs (66.9 wt%), exhibiting the highest CO evolution rate (5.2 μmol·g −1 ·h −1 ) under visible light irradiation without any sacrificial agent or photosensitizer in water. This is 26.8- and 20.9-fold higher than those of the pristine LDH , pure CN, and their binary counterparts, respectively, and also outperforms most reported LDH-based photocatalysts. As unhindered electron conduction bridges, the highly dispersed CQDs in the LDH/CN heterojunction significantly increase utilization efficiency of light energy and separation efficiency of photogenerated electron-hole pairs. This work provides a beneficial attempt to integrate CQDs with LDH/CN for the positive synergetic effect on both photoelectric properties and electron transfer to obtain highly enhanced photocatalytic activity of CO 2 into CO, and expected to be extended towards broader photocatalytic applications.
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高影响因子
Applied Catalysis O: Open
·
2024
·
IF 0
Yongsi Jiao,Cunjun Li,Yanqi Xu,Limei He,Linjiang Wang
Photodegradation of indigo carmine (IC) in wastewater has received much attention in recent decades. However, the current photocatalysts used for IC photodegradation suffer from an unsatisfactory efficiency due to low yield of reactive species. Herein, a P-modified biochar/g-C 3 N 4 (P-BC/CN) photocatalyst was fabricated by mechanochemical method using P-modified biochar and g-C 3 N 4 as precursors. It is discovered that P N bonds were constructed between P-modified biochar and g-C 3 N 4 , and these bonds served as the active sites to promote the generation of •O 2 − during the photodegradation process. The biochar component in P-BC/CN composite is conducive to transfer the photogenerated carriers, thereby avoiding their recombination. The photodegradation experiment showed that the P-BC/CN composite exhibits an impressive photodegradation performance towards IC ( C 0 = 50 mg/L) with a photodegradation rate of 95.3% in 120 min. This work provides a green and efficient method to design biochar-based photocatalyst with P N active sites for advanced wastewater purification.
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