Nanomaterials
·
2021
·Vol. 11
·期 12
·3266
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IF 5.076
Yang Li,Yue Lu,Zhaoyu Ma,Lianqing Dong,Xiaofang Jia,Junying Zhang
Graphitic carbon nitride (g-C3N4) has been widely studied as a photocatalyst for the splitting of water to produce hydrogen. In order to solve the problems of limited number of active sites and serious recombination rate of charge-carriers, noble metals are needed as cocatalysts. Here, we selectively anchored Pt nanoparticles (NPs) to specific nitrogen species on the surface of g-C3N4via heat treatment in argon–hydrogen gas mixture, thus achieving g-C3N4photocatalyst anchored by highly dispersed homogeneous Pt NPs with the co-existed metallic Pt0and Pt2+species. The synergistic effect of highly dispersed metallic Pt0and Pt2+species makes the catalyst exhibit excellent photocatalytic performance. Under the full-spectrum solar light irradiation, the photocatalytic hydrogen production rate of the photocatalyst is up to 18.67 mmol·g−1·h−1, which is 5.1 times of the catalyst prepared by non-selective deposition of Pt NPs.Keywords:graphitic carbon nitride;platinum;selective deposition;photocatalytic hydrogen production
研究领域:
材料科学
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化学工程
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DOI
PubMed
高影响因子
Journal of Environmental Chemical Engineering
·
2024
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IF 7.4
Zhilong Zhang,Lushao Gong,Xingyu Zhan,Bo Hong,Xinqing Wang,Yingchun Xia,Yunxiong Zeng
Silver phosphate (Ag 3 PO 4 ) is a promising photocatalyst, but the photo-corrosion issue limits an effective and comprehensive photocatalysis degradation of tetracycline (TC). In this work, a unique graphitic carbon nitride-Ag 3 PO 4 (KCN-AP (40 %) ) core-shell structure was prepared via a simple chemical sedimentation method. The unique graphitic carbon nitride sheet encloses Ag 3 PO 4 to trap excited electrons from the conduction band position of Ag 3 PO 4 , suppressing the reduction of Ag + and Ag metal deposition on the surface of Ag 3 PO 4 . Under visible light irradiation, the optimized KCN-AP (40 %) can photodegrade nearby 100 % of TC within 20 min with a first-order kinetic constant of 0.127 min −1, which is 3.34 and 3.97-folds higher than those of Ag 3 PO 4 and graphitic carbon nitride, respectively. A series of factors that may affect photoactivity of KCN-AP (40 %) including pH, inorganic ions, and organic matter are investigated. In final, the photodegradation mechanisms and intermediates were proposed based on ex-situ HPLC-MS. This work explains the deep decomposition of TC and presents a facile approach for designing and manufacturing Ag 3 PO 4 based nanohybrids.
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
CHEMICAL ENGINEERING JOURNAL
·
2024
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IF 13.3
Huagen Liang,Anhu Wang,Ruolin Cheng,Fu Chen,Palanisamy Kannan,Costas Molochas,Panagiotis Tsiakaras
The emerging photocatalytic production of hydrogen peroxide (H 2 O 2 ) using graphitic carbon nitride (g-C 3 N 4 ) has attracted a lot of attention for its potential applications in various fields. However, However, the catalytic activity of pure g-C 3 N 4 is still limited. Herein, Bi, K co-doped g-C 3 N 4 (Bi x K y -CN) was prepared by co-thermal polymerization of a mixture of potassium nitrate, bismuth nitrate, melamine, and urea. The obtained Bi 3.6 K 3 -CN composite possesses more negative conduction and valence band positions that can, to some extent, enhance photocatalytic performance by lowering the energy barrier of redox reactions and by enhancing electron absorption capacity. Additionally, the pyrolysis process of the potassium nitrate and bismuth nitrate has a considerable impact on the formation of the morphology of g-C 3 N 4 , generating a porous lamellar-structure with nitrogen defects, resulting in increased oxygen adsorption and utilization capacity. These synergistic effects enable Bi 3.6 K 3 -CN to exhibit excellent photocatalytic activity and cycling stability for H 2 O 2 production. After 3 hours of visible light irradiation, the production of H 2 O 2 catalyzed by Bi 3.6 K 3 -CN can reach 1207.72 μmol L -1 , which is 57 times higher than that of pure g-C 3 N 4 .
研究领域:
材料科学
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环境科学
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DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2017
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IF 9.446
Jing Ding,Wei Xu,Hui Wan,Dashui Yuan,Chong Chen,Lei Wang,Guofeng Guan,Wei-Lin Dai
Vacancy defect in the semiconductors plays an important role in the improvement of the electronic structure and the increase of specific reaction sites for reactant molecules, and consequently enhancing the photocatalytic activity of semiconductor photocatalysts. Through high-temperature thermal condensation of a nitric acid-pretreated melamine precursor, nitrogen vacancies were successfully introduced in the framework of g-C 3 N 4 . The nitrogen vacancies located at the uncondensed terminal NH x lattice sites were conducive to the enhancement of optical absorption, the improvement of the separation efficiency of the photogenerated charge carrier and the increase of surface area, which was beneficial to the photocatalytic oxidation process. More significantly, the novel CNNA(X) were used as efficient photocatalysts in the green process of aromatic aldehydes from the photocatalytic selective oxidation of aromatic alcohols and the photocatalytic degradation of organic pollutants. CNNA(X) samples exhibited enhanced photocatalytic activity and excellent recyclability and stability. The 68.3% benzyl alcohol conversion and almost 100% selectivity was observed for the CNNA (0.9) photocatalyst, higher than that of pure g-C 3 N 4 . Meanwhile, CNNA (0.9) showed superior photocatalytic degradation performance of organic dyes (RhB and MO). Furthermore, the underlying photocatalytic oxidation mechanism was proposed by the controlled experiments using radical scavengers.
研究领域:
材料科学
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环境科学
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化学工程
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DOI
高影响因子
Catalysts
·
2023
·Vol. 13
·期 3
·619
·
IF 3.9
Chen Yang,Xuefeng Hu,Yaxing Bai,Beichuan Cai,Yujie Li
In this study, a simple and low-energy synthesis scheme of Fe single-atom anchored carbon nitride was reported to improve the photocatalytic performance of g-C3N4. Synthesized Fe single-atom doped graphite carbon nitride (Fe-SACs/g-C3N4) showed high activity and stability for the degradation of 2-mercaptobenzothiazole (MBT); under visible light irradiation, 99% of MBT could be degraded within 35 min, and the degradation ability basically did not decline after five cycles, mainly due to the synergistic effect of the Fe single atoms and carbon nitride. The results of X-ray absorption fine structure (EXAFS), X-ray photoelectron spectroscopy (XPS), and density functional theory calculations show that the single-atom Fe forms Fe-N4coordination with pyridine nitrogen to generate a new electron transfer channel, which can significantly improve the in-plane separation and transfer of carriers, finally enhancing the generation of superoxide radicals. This is confirmed by time-resolved photoluminescence, photoelectron chemistry, and electron spin resonance measurements. The main intermediates of MBT degradation were determined using a liquid chromatograph–mass spectrometer (LC-MS), and a possible photocatalytic mechanism based on the quenching experiment and electron paramagnetic resonance (EPR) test was proposed. A deep understanding of the contribution of Fe single-atom sites with clear local coordination structures will help to design effective catalysts for photocatalytic performance.Keywords:graphitic carbon nitride;single-atom;NaBH4reduction;photocatalytic degradation
研究领域:
材料科学
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环境科学
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DOI
高影响因子
JOURNAL OF MOLECULAR STRUCTURE
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2023
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IF 3.8
Xin Yan,Na Zhang,Zhiliang Liu,Chunfang Du
In this paper, 1T/2H mixed-phase MoS 2 /g-C 3 N 4 composites (1T/2H-MG) were successfully synthesized by a simple two-step calcination method and used for Cr(VI) removal from aqueous environment. A series of characterization methods were used to characterize the microstructure and surface morphology of the prepared materials. The experiment results showed that 1T/2H-MG (1:12) composite with good pH and temperature adaptability could completely remove Cr(VI) (100 mg∙L –1 ) within 50 min and showed an excellent adsorption capacity of 342.06 mg∙g –1 . The presence of abundant sulfur defects in 1T/2H-MG composite could provide more adsorption and reduction active sites, which was the main reason for the enhanced removal efficiency of 1T/2H-MG in comparison with pure MoS 2 and g-C 3 N 4 . This work not only contributes an excellent adsorbent for the wastewater treatment, but also provides evidences for the defects engineering.
研究领域:
环境科学
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材料科学
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2021
·
IF 13.273
Li Lei,Qiuxia Tu,Ling Jiao,Song Xiang,Li Wang,Xia Ran,Bo Xiao,Guangwei Feng,Jian Feng,Chunlin Zhang
Mitochondrial damage mediated by reactive oxygen species (ROS) is a major contributory factor to Parkinson’s disease (PD) pathogenesis. The use of hemin-based nanomaterials to control ROS production can protect against neurological damage. Here, we report the rational design of a uniform and water-soluble artificial nanozyme based on an ultrathin graphitic carbon nitride (g-C 3 N 4 ) nanosheet with loaded hemin to reduce ROS and treat PD. The g-C 3 N 4 not only acted as a scaffold for hemin loading but also improved the stability, cytotoxicity, and catalytic action of hemin. The integration of g-C 3 N 4 increased hemin’s peroxidase activity by 31.7%, promoting effective oxidation of the substrate 3,3′,5,5′-tetramethybenzichne (TMB) in the presence of H 2 O 2 to a blue-colored solution after 10 min’ incubation at room temperature. Moreover, CN-hemin exhibited good biocompatibility and could effectively scavenge intracellular ROS and reduce cytotoxicity induced by H 2 O 2 and 6-hydroxydopamine (6-OHDA). In vivo animal studies using nematode transgenic hus111 strain and 6-OHDA pretreated C. elegan s wild-type Bristol (N2) as models further showed that CN-hemin extended their lifespan and restored dopamine-dependent behaviors such as area-restricted searching, ethanol avoidance, and the basal slowing response by reducing ROS-mediated neurotoxicity. Nanomaterials using CN-hemin enzyme mimicry have potential biomedical applications, including the treatment of PD and disorders related to ROS metabolism.
研究领域:
神经科学
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生物医学工程
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材料科学
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DOI
高影响因子
JOURNAL OF APPLIED PHYSICS
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2022
·Vol. 132
·期 18
·
IF 2.877
Zheng Xiaochun,Ren Shoutian,Gai Qixiao,Wang Yidi,Liu Wenjun
Various defects of nanocomposites inevitably bring some harmful effects on their photoelectric performance, especially considering that interface defects seriously hinder the carrier interfacial transfer. Here, the interface optimization can be realized between graphitic carbon nitride (C 3 N 4 ) and CoP co-catalyst by the introduction of good conductive carbon nanosheets (CNs). As a result, the defect density of synthesized C 3 N 4 /CNs/CoP is reduced to 1.40 × 10 12 cm −3 from 2.55 × 10 12 cm −3 of C 3 N 4 /CoP, and its interface impedance is correspondingly reduced to 34% of that of C 3 N 4 /CoP. Therefore, the optimal H 2 evolution rate of 5.26 mmol g −1 h −1 and apparent quantum efficiency of 9.27% at 420 nm are realized, which are 4.8 and 8.1 times that of C 3 N 4 /CoP photocatalyst in the absence of CNs, respectively. This work provides a general solution to reduce defect density and carrier transfer resistance in nanocomposites by the introduction of a highly conductive buffer layer.
研究领域:
材料科学
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光催化
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能源科学
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DOI
高影响因子
Cell Reports Physical Science
·
2022
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IF 7.832
Yang Ding,Soumyajit Maitra,Daniel Arenas Esteban,Sara Bals,Henk Vrielinck,Tarek Barakat,Subhasis Roy,Gustaaf Van Tendeloo,Jing Liu,Yu Li,Alexandru Vlad,Bao-Lian Su
Artificial photosynthesis of H 2 O 2 , an environmentally friendly oxidant and a clean fuel, holds great promise. However, improving its efficiency and stability for industrial implementation remains highly challenging. Here, we report the visible-light H 2 O 2 artificial photosynthesis by digging pro-superoxide radical carbon vacancies in three-dimensional hierarchical porous g-C 3 N 4 through a simple hydrolysis-freeze-drying-thermal treatment. A significant electronic structure change is revealed upon the implantation of carbon vacancies, broadening visible-light absorption and facilitating the photogenerated charge separation. The strong electron affinity of the carbon vacancies promotes superoxide radical ( ⋅ O 2 − ) formation, significantly boosting the H 2 O 2 photocatalytic production. The developed photocatalyst shows an H 2 O 2 evolution rate of 6287.5 μM g −1 h −1 under visible-light irradiation with a long cycling stability being the best-performing photocatalyst among all reported g-C 3 N 4 -based systems. Our work provides fundamental insight into highly active and stable photocatalysts with great potential for safe industrial H 2 O 2 production.
研究领域:
材料科学
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环境科学
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化学
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DOI
PubMed
高影响因子
JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
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2020
·
IF 6.155
Xiangang Lin,Xiaojuan Hou,Lixia Cui,Shiqiang Zhao,Hong Bi,Haiwei Du,Yupeng Yuan
Increasing the availability of π-electron in graphitic carbon nitride (g-C 3 N 4 ) can reduce the band gap and thus enhance the photocatalytic hydrogen (H 2 ) generation activity upon exposure to visible light. However, such strategy has not yet been largely applied to increase the H 2 generation of g-C 3 N 4 . Herein, we successfully increased the amount of π-electron in g-C 3 N 4 by incorporating π-electron-rich benzene rings through copolymerization of melamine and trimesic acid in air. The incorporation of benzene rings not only extends the light absorption of g-C 3 N 4 to 650 nm, but also improves the electrical conductivity due to delocalization of π electrons in benzene rings. As a result, a 3.4 times enhancement of photocatalytic H 2 generation was achieved from the g-C 3 N 4 with benzene ring incorporation in comparing with that of pristine g-C 3 N 4 . More interestingly, H 2 generation still occurs under irradiation of the light of λ ≥ 490 nm, above the absorption edge of pristine g-C 3 N 4 (∼ 460 nm), illustrating the positive effectiveness of incorporated benzene rings on enhancing the H 2 generation capacity of g-C 3 N 4 . The present work manifests the advantages of increasing π-conjugated electrons on designing highly active g-C 3 N 4 photocatalysts.
研究领域:
材料科学
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能源化学
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DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2024
·
IF 6.3
Dexu Zhang,Xiaoying Peng,Jie Zhang,Shixuan Zhu,Zhihong Xue,Shubin Xiong,Shuai Xiong,Bo Sheng,Yiqiang He,Guiming Peng,Jiadong Zhang
Graphitic carbon nitride (g-C 3 N 4 ) has become a favored universal photocatalyst. Despite its numerous advantages, the photocatalytic efficiency of g-C 3 N 4 is hindered by the substantial recombination of photoexcited charge carriers and holes. In this work, we demonstrate that Zn-doped tubular carbon nitride photocatalyst (Zn-tCN) can serve as highly efficient catalysts for H 2 O 2 photosynthesis. Mechanism studies confirm that the presence of Zn in g-C 3 N 4 prolongs the lifetimes of photogenerated carriers and inhibits their recombination, which triggers the reduction of O 2 to reaction intermediates ( O 2 − ), as supported by in situ electron paramagnetic resonance (EPR) spectroscopy. More importantly, sacrificial agent experiments coupled with in situ EPR results confirmed that the reaction mechanism involves a concerted two-electron transfer process. The optimal catalyst displays a H 2 O 2 productivity of 162.4μmol g –1 h −1 under visible-light irradiation without a sacrificial agent, which is 11.7 times higher than that of pristine g-C 3 N 4 (13.8μmol g –1 h −1 ). This work proposes a synthetic strategy for the preparation of high-performance Zn-doped g-C 3 N 4 , which offers insights and perspectives for developing highly active photocatalysts and deepening the understanding of photocatalytic mechanisms.
研究领域:
材料科学
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环境科学
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化学
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DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
·
IF 9.4
Huagen Liang,Haoran Wang,Anhu Wang,Ruolin Cheng,Shengyu Jing,Fu Chen,Palanisamy Kannan,Georgia Balkourani,Panagiotis Tsiakaras
Graphitic phase carbon nitride (g-C 3 N 5 ), as a novel n -type metal-free material, is employed as a visible light-receptive catalyst because of its narrow band gap and abundant nitrogen. To overcome the low carrier mobility efficiency of g-C 3 N 5 , its modification by K ions was adopted. In addition, In 2 S 3 was selected to couple with modified g-C 3 N 5 to overcome the recombination of photogenerated e − /h + . As a novel photocatalytic material, it was proven to possess a high visible light absorption capacity and a strong H 2 O 2 production ability (up to 3.89 mmol⋅L -1 in 2 h). Moreover, a S-scheme heterojunction structure was successfully constructed between the two materials, which was tested and confirmed to be successful in raising the photogenerated e − /h + separation efficiency. Ultimately, the primary processes of photocatalytic H 2 O 2 production were summarized by superoxide radical and rotating disc electron measurements. This research provides a fresh perspective for the synthesis of C 3 N 5 -based S-scheme heterojunction photocatalysts for producing H 2 O 2 .
研究领域:
材料科学
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环境科学
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产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）