Science China-Materials
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2022
·Vol. 66
·期 2
·623-633
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IF 8.64
Wang Yuqing,Si Wenping,Tan Haotian,Xie Zhiqiang,Wang Liqun,Di Lu,Liang Ji,Hou Feng
Polymeric carbon nitride (PCN) has received extensive attention in suspension photocatalysis, whereas the preparation of high-quality PCN film is still at an initial stage, limiting its practical application in photoelectrochemical (PEC) systems. Herein, an integrated molten and vapor condensation route is realized using small molecule precursors dicyandiamide (DCDA) and thiourea (TU) to form PCN film photoelectrode with high performance. The in-situ deposition route endows the PCN film with a composite structure including a thick porous zone with suitable thickness for light absorption and thin compact zone with a higher C/N ratio for better charge transportations. The growth of the specific film and the functions of precursors DCDA and TU are investigated in detail. Owing to the unique condensation route and film structure, this PCN film exhibits excellent performance in PEC water splitting with a photocurrent density of ca. 140 µA cm −2 in 0.1 mol L −1 NaOH electrolyte at 1.23 V RHE , which is competitive or higher than the results of the reported PCN photoanodes prepared by the molten-mediated method and thermal vapor condensation. The integrated molten and vapor condensation strategy is enlightening for comprehending the growth of PCN photoelectrodes.
研究领域:
材料科学
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化学工程
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能源技术
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电化学
✓ 已验证
DOI
高影响因子
CHEMOSPHERE
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2022
·
IF 8.943
Yiling He,Ming Gao,Yanbo Zhou,Yi Zhou
Antibiotic abuse will seriously affect the ecology and environment. Photocatalytic oxidation technology based on carbon nitride (g-C 3 N 4 ) has been widely adopted to treat wastewater containing antibiotics. Here, a novel composite photocatalyst MCNT was prepared by loading manganese oxide (Mn 3 O 4 ) on the surface of g-C 3 N 4 nanotubes (CNT). Three typical antibiotics, trimethoprim (TMP), norfloxacin (NOR), and tetracycline (TC) were used as model contaminants to evaluate the oxidative properties of prepared materials. Compared with bulk g-C 3 N 4 , the degradation rates of TMP, NOR, and TC catalyzed by MCNT-5 were increased by 2, 3, and 1.4 times, respectively, mainly due to 1) the larger specific surface area of the nanotube structure of CNT, which provides abundant active sites for antibiotic adsorption and catalytic oxidation, and 2) the loading of Mn 3 O 4 , which promotes the directional migration of photogenerated charges and improves the separation efficiency of photogenerated electrons and holes. The free radical capture and quenching experiments confirmed that MCNT degraded the target organic pollutants with hydroxyl radical (·OH) and singlet oxygen ( 1 O 2 ) as the main active oxidants. This catalyst maintained 80% photocatalytic oxidation performance after five cyclic experiments. This study provides new insights into developing efficient, stable, and environmentally-friendly photocatalysts and provides a new dimension to mitigate the antibiotic pollution problem.
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2025
·
IF 6.3
Xinyu Liu,Xixi Meng,Tao Zhong,Yuxin Wang,Fuying Wu,Hu Liu,Hong Li,Liuting Zhang
Magnesium hydride (MgH 2 ) with its high hydrogen storage capacity (7.6 wt%) and exceptional reversibility, has emerged as a promising solid-state hydrogen storage material. This study designed a polymeric carbon nitride (PCN) supported single-phase Ni catalyst with superior thermal stability and catalytic activity. The optimized PCN-Ni catalyst significantly reduced the initial dehydrogenation temperature of MgH 2 to 192 ºC. At 295 ºC, the composite released 6.10 wt% H 2 within 5 min, and it subsequently absorbed 5.50 wt% H 2 within 5 min at 150 ºC. Compared to pristine MgH 2 , the activation energies for dehydrogenation and hydrogen absorption were reduced by 31.6 % and 29.4 %, respectively. Moreover, the MgH 2 + 10 wt% PCN-Ni composite exhibited remarkable cycling stability, with capacity retention rates of 96.0 % and 96.7 % after 20 hydrogenation/dehydrogenation cycles. In conclusion, this work provides a new perspective on the heterogeneous synergy of transition metal and carbon nitride composite catalysts in promoting the dehydrogenation/rehydrogenation reactions of MgH 2 and lays the foundation for the design and fabrication of highly efficient catalysts in other energy storage related fields.
研究领域:
材料科学
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能源存储
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF CATALYSIS
·
2025
·
IF 6.5
Yixin Li,Jianhao Qiu,Jie Xu,Yong Tang,Dingliang Dai,Guanglu Xia,Biyao Fang,Jianfeng Yao
The utilization of solar energy to break the C α C β bonds in lignin under mild conditions is highly important for lignin valorization. This work presents an MIL-125-derived titanium oxide (M-TiO 2 )-modified carbon nitride (g-C 3 N 4 ) heterostructure for selective photocatalytic lignin C α C β bond cleavage at room temperature. The conversion of lignin model 2-phenoxy-1-phenylethanol (PP-ol) reached 90.8 % over M-TiO 2 /g-C 3 N 4 composites, which is visibly higher than that of bare M-TiO 2 (33.2 %) and g-C 3 N 4 (57.3 %). Furthermore, the selectivity of C α C β bond breakage reached 96.8 %, and the yield of benzaldehyde was as high as 86.4 %. A mechanistic study innovatively demonstrated that lignin C α C β bond cleavages are achieved by the cooperative effect between holes and 1 O 2 , where holes dominate PP-ol conversion, whereas 1 O 2 governs C α C β bond cleavages. M-TiO 2 has relatively large surface areas and high porosities, and the Z-scheme heterojunctions retard charge carrier recombination and outfit strong redox abilities, which separately prompt O 2 adsorption and evolution to generate 1 O 2 , accounting for the high selectivity of C α C β bond breakages over M-TiO 2 /g-C 3 N 4 composites. This study sheds new light on the potential of metal–organic framework-derived materials in photocatalysis and provides valuable insights into the photocatalytic cleavage of lignin C α C β bonds.
研究领域:
材料科学
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环境科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
ENVIRONMENTAL TECHNOLOGY
·
2022
·
IF 3.475
Yafang Zhang,Shuning Yang,Linsheng Wei,Xiaoyang Zhao,Xiangdong Lu
Photocatalysis is a promising technology for wastewater treatment. It is of great significance to find catalysts with high photoactivity. In this paper, a catalyst with high photocatalytic degradation efficiency to organic wastewater, carbon nitride modified by graphene quantum dots (SCN-GQDX), is prepared by supramolecular self-assembly thermal polycondensation method and doping graphene quantum dots (GQDs). The results show that SCN-GQD0.5 has the best catalytic performance, and its photocatalytic degradation efficiency to organic pollutants can reach 86% and still remains above 83% after five cycles, which shows the modified carbon nitride has high catalytic efficiency and stability. In a word, SCN-GQDX is a highly efficient, non-toxic and stable photocatalyst for organic pollutants in wastewater.
研究领域:
环境科学
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材料科学
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废水处理
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产品关联
DOI
PubMed
高影响因子
ChemCatChem
·
2018
·Vol. 11
·期 3
·1045-1056
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IF 4.674
Gui-Ying Zhuge,Wei-De Zhang
Graphical This study reports a strategy to tune nitrogen content in carbon nitride using isonicotinic acid as an additive in the precursors. The nitrogen-rich and nitrogen-deficient g-C 3 N 4 samples display enhanced visible light absorption and improved separation of charge carriers, and thus the high hydrogen evolution rate. Graphitic carbon nitride (CN) with various nitrogen contents can be prepared to regulate its electronic structure and energy band levels. The newly-prepared graphitic carbon nitride manifests high photocatalytic activity. In this work, nitrogen-rich CN (CN-NR100) and nitrogen-deficient CN (CN-ND500) were prepared by tuning nitrogen contents in CN while using isonicotinic acid (IA) as an additive in the precursors. It is found that IA reacting with urea can introduce its nitrogen to CN, while reacting with CN can take away the amino group of CN, thus reduces its nitrogen content. Interestingly, the gas that comes from the decomposition of IA is essential for the formation of porous morphology in CN. Both CN-NR100 and CN-ND500 can provide more photocatalytic sites, narrow bandgaps to enhance the absorption of visible light and significantly improve the charge carrier separation efficiency. Therefore, CN-NR100 and CN-ND500 manifest an excellent photocatalytic hydrogen evolution rate of 73 μmol h −1 (about 4 times of that of CN) and 120 μmol h −1 (6.7 times of that of CN), respectively. This work provides an efficient strategy to prepare CN with different nitrogen contents by pyrolysis of precursors modified by IA for high photocatalytic hydrogen evolution.
研究领域:
材料科学
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光化学
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催化
✓ 已验证
产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
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2025
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IF 6.9
Yangjie Fu,Jiurui Chi,Yanling Wu,Jun Li,Meng Tan,Chunjuan Li,Hao Du,Derek Hao,Huayue Zhu,Qi Wang,Qiang Li
Constructing a robust and large built-in electric field to boost photogenerated carrier separation efficiency has been a persistent challenge in photocatalysis. Herein, a carbon-rich carbon nitride (CCN/WO 3 ) S-scheme heterojunction was successfully developed, achieving effective charge separation through the synergistic interaction of the in-plane electric field within CCN and the interfacial electric field at the CCN/WO 3 interface. The robust in-plane electric field of CCN originated from the asymmetric structure induced by carbon substitution for nitrogen atoms in g-C 3 N 4 . Additionally, a strong interfacial electric field was established through combining CCN with WO 3 via a one-pot synthesis process. The CCN/WO 3 heterojunction demonstrated excellent performance in bacteria inactivation and organic pollutant degradation, with antibacterial activity against E. coli 20.4 times and 4.2 times higher than those of WO 3 and CN/WO 3 , respectively, and a photocatalytic TC degradation rate constant 5.5 times higher than that of WO 3 . Quantitative analysis revealed that the CCN/WO 3 heterojunction achieved 96.7 % selectivity for free radical generation, significantly higher than that of g-C 3 N 4 (40.9 %), indicating a strong preference for activating O 2 through charge-carrier transfer pathways. This study demonstrates that leveraging the synergy between in-plane and interfacial electric fields offers a promising strategy to enhance charge separation in photocatalysts.
研究领域:
环境科学
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材料科学
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化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF MOLECULAR STRUCTURE
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2024
·
IF 4
Lingmin Wu,Baitao Li
The present study assessed the catalytic performance in epoxidation of styrene using tert ‑butyl hydroperoxide (TBHP) as an oxidant over single-atomic copper-doped Ordered mesoporous alumina (Cu-OMA) composited with g -C 3 N 4 (CN). The thermal treatment at three temperatures (300, 500, 700 °C) provided a facile mean to modify the texture and electronic structure of the Cu-OMA@CN composite. The X-Ray absorption spectroscopy proved the single-atomic Cu-O-Al and Cu-O-C in Cu-OMA@CN-500 catalyst. Catalytic reaction parameters, namely temperature (60–80 °C), catalyst amount (10–70 mg), substrate/oxidant ratio (1:1–1:3), and solvents (acetone, ethanol, acetonitrile, N, N-dimethylacetamide) were optimized to obtain high conversion of styrene and selectivity to styrene epoxide. Under the optimized reaction conditions (75 °C, 30 mg of catalyst, 1:2 of styrene/TBHP and acetonitrile as solvent), the conversion decreased in the order of Cu-OMA@CN-500 > Cu-OMA@CN-300 > Cu-OMA@CN-700. This sequence was related to the formation of electron-rich single-atom copper sites, high surface area, medium alkaline environment and high content of graphic nitrogen species in Cu-OMA@CN-500. This structure differed from the blocky structure of C 3 N 4 in Cu-OMA@CN-300 and the destroyed tri-s-triazine ring in Cu-OMA@CN-700. The most active Cu-OMA@CN-500 catalyst displayed a high styrene conversion (87.2 %) and striking selectivity to styrene oxide (90.0 %). Its catalytic activity was retained after five recyclability tests. The possible catalytic mechanism for epoxidation of styrene over this catalyst was tentatively proposed.
研究领域:
催化化学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
Water
·
2022
·Vol. 14
·期 16
·2569
·
IF 3.53
Weifan Gao,Guichang Zhang,Xiaoping Zhang,Shaoqi Zhou,Zihao Wang
The catalytic capability of original carbon nitride (CN) is limited by a small specific surface area and high electron–hole recombination rate. In this study, WO3-loaded porous carbon nanosheets (MCA-CN/WO3) were synthesized by thermal treatment with melamine, cyanuric acid and WCl6. The MCA-CN/WO3could degrade 98% of the methylene blue (MB) within 30 min in the photo-Fenton-like process, displaying better catalytic activity than the original CN (30%), pure MCA-CN (63%) and original CN/WO3(87%). The results of photoluminescence and electrochemical impedance spectroscopy demonstrated that the Z-scheme heterojunction of MCA-CN/WO3inhibited the recombination of electrons and holes. In addition, the porous nanosheet structure accelerated the electron transfer and provided abundant active sites for MB degradation. A radical quenching experiment indicated that the Z-scheme heterojunction facilitated the decomposition of H2O2to produce1O2for MB degradation. The possible degradation pathways of MB were proposed.Keywords:photo-Fenton-like process;WO3-loaded porous carbon nitride nanosheet;Z-scheme heterojunction;MB degradation
研究领域:
环境科学
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材料科学
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产品关联
DOI
高影响因子
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
·
2023
·Vol. 25
·期 18
·12754-12766
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IF 3.3
Qixiao Gai,Shoutian Ren,Xiaochun Zheng,Wenjun Liu
Cu nanoparticles (NPs) are low-cost surface plasmonic resonance (SPR) metal nanostructures, and their SPR properties can be used to enhance the photocatalytic hydrogen evolution performance of carbon nitride (C3N4). But their actual performance is usually limited, and one key factor is their poor interfacial quality. In this work, a highly conductive reduced graphene oxide (RGO) interlayer is introduced between protonated C3N4 (PCN) nanosheets and Cu NPs, which can act as an efficient sink for photogenerated electrons from C3N4 and hot electrons from Cu NPs, and simultaneously serve as reaction sites for the hydrogen evolution reaction, and accelerate the charge transport by the formed C–O–C and C–O–Cu bonds. The optimal hydrogen evolution rate of the optimized PCN/RGO/Cu is 1.30 mmol g−1 h−1, which is 6.76, 2.47 and 2.41 times that of PCN, PCN/RGO and PCN/Cu, respectively, and it can further reach up to 13.22 mmol g−1 h−1 by loading moderate Pt NPs. Meanwhile, the introduced RGO can effectively anchor Cu NPs to enhance the stability of the photocatalyst. In addition, due to the broad SPR response of Cu NPs, a near-infrared photocatalytic performance is realized for PCN/RGO/Cu with an apparent quantum efficiency of 0.46% at 765 nm.
研究领域:
材料科学
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光催化
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纳米技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2023
·
IF 7.2
Fang He,Hong Zhong,Meng Wang,Hubo Yuan,Zhenxing Wang,Shaoqin Peng,Yuexiang Li
All carbon-based CG/M − CN rectangular nanotubes have been constructed by a facile molten salt thermal condensation of melamine and glucose. In the molten salt fluid, the glucose is carbonized into graphene-like (CG) nanosheets acting as an electron acceptor , and the melamine thermally condenses into carbon nitride (M − CN) rectangular nanotube acting as an electron donor . The 0.5 wt% CG/M − CN nanotubes display a photocatalytic H 2 evolution rate of 2345 μmol h −1 g −1 , which is 1.52 times higher than that of M-CN. Moreover, without loading Pt co-catalyst, the 0.5 wt% CG/M − CN nanotubes show a 12.75 times higher photocatalytic H 2 evolution rate than that of M-CN. It is revealed that the graphene-like CG nanosheets not only can act as an electron acceptor boosting charge carrier separation, but also function as a HER cocatalyst for M-CN. Our work provides a new insight for the development of all carbon-based photocatalysts for energy-related applications.
研究领域:
材料科学
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能源科学
✓ 已验证
产品关联
DOI
高影响因子
Nano-Micro Letters
·
2023
·Vol. 15
·期 1
·1-13
·
IF 26.6
Gao Manyi,Tian Fenyang,Zhang Xin,Chen Zhaoyu,Yang Weiwei,Yu Yongsheng
A hybrid co-catalysts system comprising Au nanoparticles (NPs) and PtSAs with different functions was constructed on the polymeric carbon nitride (PCN) surface by double-solvent method.
For the dual co-catalysts, the Au NPs absorb relatively long-wavelength light to produce plasmonic hot-electrons, and the adjacent Pt single atoms (PtSAs) can trap the plasmonic hot-electrons effectively for H 2 evolution.
The PtSAs–Au 2.5 /PCN exhibits excellent broad-spectrum photocatalytic H 2 evolution activity with the H 2 evolution rate of 8.8 mmol g − 1 h − 1 at 420 nm and 264 μmol g − 1 h − 1 at 550 nm, respectively.
研究领域:
纳米技术
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光催化
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材料科学
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等离激元学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）