JOURNAL OF HAZARDOUS MATERIALS
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2019
·
IF 7.65
Lu-Lu Qu,Zhi-Qin Geng,Wen Wang,Kai-Chun Yang,Wei-Peng Wang,Cai-Qin Han,Guo-Hai Yang,Robert Vajtai,Da-Wei Li,Pulickel M. Ajayan
A three-dimensional (3D) substrate was developed by assembling a monolayer of graphitic carbon nitride (O-g-C 3 N 4 ) on Ag nanorod arrays (Ag NRs) for sensitive and recyclable surface enhanced Raman scattering (SERS) detection. The prepared Ag NRs/O-g-C 3 N 4 substrate not only generated a significant Raman enhancement effect as a result of the strong π-π stacking interaction between O-g-C 3 N 4 and the analytes but also possessed excellent self-cleaning property via visible-light irradiation that was attributed to its outstanding catalytic performance. Highly sensitive SERS detection could be achieved with a LOD of 8.2 × 10 −10 M for R6 G, and the substrate could be used repeatedly for at least four cycles with tolerable intensity attenuation. In addition, the 3D substrate exhibited long-term stability originating from the electron-donor effect of O-g-C 3 N 4 and high reproducibility due to the uniform decoration of O-g-C 3 N 4 on the Ag NRs through the strong interaction. Furthermore, using Ag NRs/O-g-C 3 N 4 , the recyclable detection of antibiotics in a water sample was demonstrated with high sensitivity, which indicates that the 3D Ag NRs/O-g-C 3 N 4 substrate is a promising candidate for eliminating the challenges of single-use SERS substrates and building a portable SERS platform to sense organic molecular species.
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高影响因子
APPLIED SURFACE SCIENCE
·
2019
·
IF 5.155
Lingli Wang,Yu Zhu,Dan Yang,Lei Zhao,Hanming Ding,Zhaohui Wang
Effective photogenerated charge separation and rapid Cu(II)/Cu(I) redox cycling is still challenging for photocatalytic reactions and copper-based Fenton-like process, respectively. Herein, a novel heterogeneous Fenton-like catalyst of copper incorporated carbon ring- g -C 3 N 4 (Cu-C-CN) was prepared through a facile calcination method. The carbon ring could be intimately connected with g -C 3 N 4 via sp 2 -hybridized C N bonds to form an in-plane π-conjugated structure. The carbon ring spliced g -C 3 N 4 (C-CN) can serve as an effective electron-hole separator owing to the varied electron affinity of two domains (e.g. carbon-ring and g -C 3 N 4 ). The copper species were further introduced to the framework of g -C 3 N 4 via the Cu N bonds to act as acceptors of conduction-electrons from g -C 3 N 4 and H 2 O 2 activators. Taking the photodegradation of methylene blue (MB) as a model reaction, the decomposition efficiency over Cu-C-CN is 5.5 times higher than that of pristine g -C 3 N 4 , and would nearly linearly increase with pH. The notable enhancement in photodegradation efficiency could be ascribed to the synergetic collaboration between photocatalysis process and Fenton-like process to generate abundant OH and e − . The Cu-C-CN catalyst shows high recycling stability with negligible Cu leaching due to the strong affinity of Cu 2+ to g -C 3 N 4 framework. The strategy of coupling Fenton-like catalysts, electron-deficient domains (e.g. carbon-ring) into semiconductor-based photocatalysis provides a facile and promising solution to the remediation of water pollution with solar energy.
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高影响因子
APPLIED SURFACE SCIENCE
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2019
·
IF 5.155
Peng Lv,Chongyang Zhao,Woo Jae Lee,Siping Huo,Se-Hun Kwon,Jun Fang,Yang Yang
Zero-dimensional/two-dimensional (0D/2D) TiO 2 /g-C 3 N 4 heterostructural photocatalysts were fabricated via ALD technique. TiO 2 nanoparticles were “site-selectively grown” on g-C 3 N 4 nanosheets and the surface modification induced band engineering of the composite photocatalysts. Thus, the redox properties of the photocatalysts were fine tuned. Under visible light , since only g-C 3 N 4 was excited, TiO 2 was acting as the electron transport channel in the optimized interfacial structures . They effectively suppressed the recombination and facilitated the transfer of photogenerated charges, improving the photocatalytic activity. When both the components were excited under UV–vis light, the dynamic equilibrium of the conduction band positions on these n–n type semiconductor heterojunctions led to the increased recombination rate of charges, decreasing the reactivity for H 2 evolution. However, the photocatalytic degradation of organic pollutants by these composite photocatalysts exhibited enhanced activities, resulting from the photogenerated holes on VB of TiO 2 which could promote oxidation of organic pollutants with strong oxidation potentials. Furthermore, TiO 2 /g-C 3 N 4 photocatalysts with limited numbers of deposition cycles exhibited optimal photocatalytic activity under visible light. In contrast, excessive deposition cycles on g-C 3 N 4 for TiO 2 /g-C 3 N 4 led to continuous film and increased thickness of TiO 2 , resulting in the attenuation of the reactivity. We verified this TiO 2 /g-C 3 N 4 photocatalysts with less mass-loading, but more enhanced photocatalytic activity.
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高影响因子
APPLIED SURFACE SCIENCE
·
2019
·
IF 5.155
Xue-Chun Yang,Yun-Ling Yang,Shao-Lin Zhang,Yu-Feng Liu,Si-Jie Fu,Meng Zhu,Jian-Feng Hu,Zhi-Jun Zhang,Jing-Tai Zhao
A novel porous nitrogen doped carbon dots (NCDs)@g-C 3 N 4 composite was successfully synthesized by a facile hydrothermal approach. The surface area of NCDs@g-C 3 N 4 can reach up to 60.9 m 3 /g, and pores with diameter between 20–50 nm are the most widely distributed. The photocatalytic activity of NCDs@g-C 3 N 4 toward the degradation of Methylene blue (MB) under visible light irradiation was remarkably higher than that of g-C 3 N 4 and NCDs. The improved photocatalytic activity can be attributed to the fact that the addition of NCDs not only broadens the photo-response range, but also suppresses the photo-generated electrons and holes recombination of g-C 3 N 4 . Degradation rate of 2.0 wt% NCDs@g-C 3 N 4 is about twice than that of pristine g-C 3 N 4 at 60 min under the same conditions. In addition, at 120 min, MB was almost degraded completely by 2.0 wt% NCDs@g-C 3 N 4 with the degradation rate as high as 97.9%, while the pristine g-C 3 N 4 was only 69%. NCDs@g-C 3 N 4 can be used as a potential catalyst for organic contaminants degradation considering its high photo-response range and excellent photocatalytic activity. Moreover, NCDs, g-C 3 N 4 and NCDs@g-C 3 N 4 also can be used as fluorescent inks for anti-counterfeiting.
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JOURNAL OF MATERIALS SCIENCE
·
2019
·Vol. 55
·期 10
·4358-4371
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IF 3.442
Zhu Zhi,Ma Changchang,Yu Kesheng,Lu Ziyang,Liu Zhi,Yan Yongsheng,Tang Xu,Huo Pengwei
It is still a challenging work to realize the universality of photocatalytic materials for unselectively removing environmental pollutants in water. Here, a ternary magnetism CoFe 2 O 4 /g-C 3 N 4 /HNTs heterojunction photocatalyst is firstly prepared, and the morphology, crystalline property, surface area, and magnetic recycling capability of the photocatalyst were investigated. The CoFe 2 O 4 /g-C 3 N 4 /HNTs shows a superior degradation efficiency for degrading 2-mercaptobenzothiazole (MBT) than that of pure g-C 3 N 4 . The high degradation performance that derives from the hollow structure of halloysite nanotubes (HNTs) can inhibit stacking of g-C 3 N 4 , which results in a larger specific surface area and more abundant reaction sites. Meanwhile, the heterojunction structure between g-C 3 N 4 and CoFe 2 O 4 improved the separation efficiency of charge carriers. In addition, the intermediate products, degradation pathway, and reaction mechanism of representative MBT pollutant over the CoFe 2 O 4 /g-C 3 N 4 /HNTs photocatalyst are revealed in depth. This work makes an important development.
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高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2019
·
IF 4.084
Yue Sun,Simeng Shao,Yanfeng Wang,Wenjuan Lu,Pingping Zhang,Qingqiang Yao
For the first time, g-C 3 N 4 @α-Fe 2 O 3 /Co-Pi heterojunctional hollow spheres were successfully fabricated via thermal condensation method followed by solvothermal and photo-deposition treatment, which showed excellent photocatalytical property. Except for the Z-scheme charge transfer between α-Fe 2 O 3 and g-C 3 N 4 , the Co-Pi could further reduce the combination of photogenerated electrons and holes as a hole storage agent, resulting in remarkably enhanced visible-light photocatalytic water splitting activity with the H 2 production rate of 450 μmol h −1 g −1 , which is 15.7 times higher than that of g-C 3 N 4 . Moreover, the photocatalytic activity of the prepared ternary hollow photocatalysts showed almost no significant weakness after five cycles, which indicated their good performance stability. The as-prepared g-C 3 N 4 @α-Fe 2 O 3 /Co-Pi also possessed good activity for overall water splitting with the hydrogen production rate reaching 9.8 μmol h −1 g −1 . This synthesized g-C 3 N 4 @α-Fe 2 O 3 /Co-Pi composite is expected to be a promising candidate for water splitting.
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Nanoscale Advances
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2019
·Vol. 2
·期 1
·274-285
·
IF 0
Qun Wang,Sicao Yu,Wei Qin,Xiaohong Wu
Two phase photocatalysts can be intergrown with each other, resulting in superior photocatalytic properties. Herein, methylamine lead bromide (MAPbBr3) wrapped/entrapped protonated graphitic carbon nitride (p-g-C3N4) intergrowth microcrystals were fabricated by mixing a pervoskite precursor with p-g-C3N4 colloidal sol. A highly stable isopropanol (IPA) solvent based photocatalytic system for dye degradation was demonstrated. The composite with an optimal p-g-C3N4 mass percentage of 3.3 wt% (denoted as MAPbBr3/p-g-C3N4-1.0 mg) exhibited the highest photocatalytic degradation of malachite green (99.8%) within 10 min under visible light, which was 5.3-fold and 16-fold greater than that exhibited by its constituents separately. The strong chemical interaction and fundamental photophysical processes in MAPbBr3/p-g-C3N4 were systematically evaluated by spectroscopic and electrochemical techniques, confirming the effective separation of photogenerated electron–hole pairs and faster interfacial charge transfer behavior. Furthermore, active superoxide radicals (O2˙−) played a vital role in the catalytic reaction, because of the significant photoinduced electron transfer rate (ket) in the inverted type-I core/shell MAPbBr3/p-g-C3N4 band configuration structure. In addition, MAPbBr3/p-g-C3N4 has good cycling stability for 10 cycles and versatility for other cationic (RhB) and anionic (MO) dye pollutants, indicating the great potential for solar energy conversion into chemical energy.
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MICROCHIMICA ACTA
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2019
·Vol. 186
·期 11
·1-8
·
IF 5.479
Duan Wei,Yan Pengcheng,Dong Jintao,Chen Yun,He Xiaoyang,Chen Jianping,Qian Junchao,Xu Li,Li Henan
A self-powered photoelectrochemical (PEC) aptamer probe is presented for the determination of oxytetracycline (OTC). The assay is based on the use of g-C 3 N 4 and NiO nanocrystals (NCs) which form a heterojunction. The latter was prepared by two-step hydrothermal pyrolysis by using the ionic liquid 1-hydroxyethyl-3-methylimidazole chloride which functions as a morphological template to form NiO NCs. The heterojunction exhibits much better electronic conductivity, wider absorption range, higher electron-hole-separation productivity, and stronger photocurrent compared to plain g-C 3 N 4 . The heterojunction was adopted to construct a self-powered PEC aptamer probe for OTC detection. An OTC-binding aptamer was immobilized on the heterojunction and the probe was constructed. The aptamer on the probe binding with OTC can form steric hindrance for transmitting of electrons and cause the PEC signal change depending on the OTC concentration. The photocurrent decreases with increasing OTC concentration in the 0.01 to 100 nM concentration range and its detection limit is 4 pM (at S/ N = 3).
Schematic representation of a self-powered photochemical aptamer probe. The probe performs enhanced ability for oxytetracycline (OTC) determination due to the formation of NiO nanocrystals/g-C 3 N 4 (NiO NCs/g-C 3 N 4 ) heterojunction and the specification recognition of the aptamer.
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ACS Sustainable Chemistry & Engineering
·
2018
·
IF 6.14
Jiajia Feng,Dingke Zhang,Hongpeng Zhou,Mingyu Pi,Xiaodeng Wang,Shijian Chen
Fabricating heterostructures to promote the charge separation and doping heteroatom to modulate the band gap of the photocatalysts have been regarded as effective strategies to improve the photocatalytic performance. However, it is still an unresolved issue of doping element and fabricating heterostructures with good contact at the same time. In this study, P nanostructures/P doped graphitic carbon nitride composites (P@P-g-C3N4) were successfully composited by a solid reaction route. Various structural characterizations, including X-ray adsorption near edge structure, indicate that P has been doped into g-C3N4 and P nanostructures were directly grown on g-C3N4 to form heterostructures. As expected, the intimate contacted heterostructured composites exhibit much enhanced light absorption and high-efficiency transfer and separation of photogenerated electron–hole pairs, and consequently, the composites also possess the superior photocatalytic performance in the rapidly degrading RhB and an efficient H2 production rate of 941.80 μmolh–1g–1. Systematical studies combining experimental measurements with theoretical calculations were carried out to expound the underlying reasons behind the distinct performance. This study pave a one-step way to synthesize earth abundant element C, N, and P as novel photocatalysts for photochemical applications.
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ChemSusChem
·
2019
·Vol. 12
·期 4
·898-907
·
IF 7.804
Dong-Dong Qin,Jing-Jing Quan,Shi-Fang Duan,Jovan San Martin,Yixiong Lin,Xiaolin Zhu,Xiao-Qiang Yao,Jin-Zhan Su,Ingrid Rodríguez-Gutiérrez,Chun-Lan Tao,Yong Yan
Graphical A single step for g-C 3 N 4 , a giant leap for water splitting : A simple phosphide gas treatment of g-C 3 N 4 coated TiO 2 -nanorod configuration not only narrows the band gap of g-C 3 N 4 by 0.57 eV into visible range but also generates a metal phosphide (M=Fe, Cu) water oxidation cocatalyst in situ. This TiO 2 /g-C 3 N 4 /FeP configuration significantly improves charge separation and transfer capability, resulting in an enhanced photoelectrochemical water oxidation. Graphitic carbon nitride (g-C 3 N 4 ) has been widely explored as a photocatalyst for water splitting. The anodic water oxidation reaction (WOR) remains a major obstacle for such processes, with issues such as low surface area of g-C 3 N 4 , poor light absorption, and low charge-transfer efficiency. In this work, such longtime concerns have been partially addressed with band gap and surface engineering of nanostructured graphitic carbon nitride (g-C 3 N 4 ). Specifically, surface area and charge-transfer efficiency are significantly enhanced through architecting g-C 3 N 4 on nanorod TiO 2 to avoid aggregation of layered g-C 3 N 4 . Moreover, a simple phosphide gas treatment of TiO 2 /g-C 3 N 4 configuration not only narrows the band gap of g-C 3 N 4 by 0.57 eV shifting it into visible range but also generates in situ a metal phosphide (M=Fe, Cu) water oxidation cocatalyst. This TiO 2 /g-C 3 N 4 /FeP configuration significantly improves charge separation and transfer capability. As a result, our non-noble-metal photoelectrochemical system yields outstanding visible light (>420 nm) photocurrent: approximately 0.3 mA cm −2 at 1.23 V and 1.1 mA cm −2 at 2.0 V versus RHE, which is the highest for a g-C 3 N 4 -based photoanode. It is expected that the TiO 2 /g-C 3 N 4 /FeP configuration synthesized by a simple phosphide gas treatment will provide new insight for producing robust g-C 3 N 4 for water oxidation.
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高影响因子
ACS Applied Materials & Interfaces
·
2018
·
IF 8.097
Lulu Qu,Gen Zhu,Jie Ji,T. P. Yadav,Yijiang Chen,Guohai Yang,Hui Xu,Haitao Li
Organic pollutants are harmful to human health, which creates a global need for the development of novel and effective materials for efficiently removing contaminants. Accordingly, an efficient visible light-driven heterostructured membrane combined with oxygen-modified monolayer g-C3N4, graphene oxide, and nitrogen-doped carbon nanotubes (CNTs) (O-g-C3N4/GO/N-CNT) was successfully fabricated through electrostatic interactions and subsequent vacuum filtration. The results suggested that the O-g-C3N4/GO/N-CNT membrane exhibited higher degradation rate than those of O-g-C3N4/GO and pure O-g-C3N4 under visible light exposure. This enhanced photocatalytic performance was attributed to the introduction of GO and N-CNT, which acted as electronic acceptors for monolayer O-g-C3N4 that effectively inhibited recombination of photogenerated electron–hole pairs, thus enhancing visible light photocatalytic activity. Furthermore, the enrichment and degradation rates of O-g-C3N4/GO/N-CNT membranes were demonstrated for tetracycline hydrochloride, which were found to be 96.64 and 94.30%, respectively, and no distinct enrichment or catalytic activity reduction was observed when their reusability was measured. These results suggested that these recyclable O-g-C3N4/GO/N-CNT membranes provide a new strategy for the highly efficient removal of environmental pollutants.
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高影响因子
Catalysis Science & Technology
·
2018
·Vol. 8
·期 11
·2853-2859
·
IF 5.365
Ya-Nan Liu,Xiao Zhou,Cong-Cong Shen,Zhi-Wei Zhao,Yi-Fan Jiang,Liu-Bo Ma,Xiao-Xiang Fang,Zeb Akif,Tuck-Yun Cheag,An-Wu Xu
Herein, a polymeric graphitic carbon nitride (for simplicity, g-C3N4) photocatalyst has been identified as a promising material for hydrogen production from water due to its comparatively low cost and facile modification of its electronic structure. However, to date, how to speed up the transfer rate of photogenerated charges, especially hole transfer rate, still remains a formidable challenge. Herein, a novel system of g-C3N4/1,1′-ferrocenedicarboxylic acid (FcDA) composites was developed for efficient visible light-driven H2 evolution, in which the redox mediator FcDA served as hole-transport molecules and platinum (Pt) acted as an electron sink. The FcDA molecules are anchored onto g-C3N4 by hydrogen-bonding interactions between the carboxylic groups and amino groups as well as π–π interactions between aromatic FcDA and graphitic C3N4. The matched energy-levels between g-C3N4 and FcDA facilitate photogenerated hole transfer from the g-C3N4 valence band to FcDA that results in the formation of FcDA+ radicals, and thus, photoinduced electrons and holes are efficiently separated. Due to the additional charge separation pathway, enhanced hole transfer kinetics, and the extremely rapid intermolecular radical reactions, charge recombination is effectively suppressed; therefore, more electrons can be released for hydrogen production. Under optimal experimental conditions, the developed g-C3N4/FcDA composite with 4 wt% FcDA exhibits high water splitting activity with a H2 evolution rate of up to 77.91 μmol h−1, which is nearly 6 times that of bare g-C3N4 (13.18 μmol h−1). Moreover, the obtained g-C3N4/FcDA photocatalyst displays excellent stability, and there is no obvious decrease in the H2-production rate after five test cycles. Thus, we anticipate that our simple modification strategy will offer an avenue to merge the polymeric g-C3N4 photocatalyst with surface organometallic chemistry for high-efficiency solar-to-fuel conversion.
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