Nano Energy
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2018
·
IF 13.12
Peng Zhou,Fan Lv,Na Li,Yelong Zhang,Zijie Mu,Yonghua Tang,Jianping Lai,Yuguang Chao,Mingchuan Luo,Fei Lin,Jinhui Zhou,Dong Su,Shaojun Guo
Tuning reactive metal-support interaction (RMSI) is a promising approach to optimizing catalytic active sites via the electronic, geometric and compositional effects. In general, the RMSI is conducted on the reducible oxides via a high-temperature reaction (>550 °C). Herein we report a strong RMSI between Pt single atom (PtSA) and non-oxide-based g -C 3 N 4 built by an in-situ photocatalytic reduction method at a sub-zero temperature. The experimental observation confirms that the rich N vacancies in g -C 3 N 4 produce an obvious electron-deficient effect, which greatly enhances the RMSI. This strong RMSI contributes to the highest PtSA coverage density of 0.35 mg m −2 reported to date in carbon-based materials and outstanding H 2 -evolution activity of 174.5 mmol g −1 h −1 per PtSA relative to those on the electron-rich g -C 3 N 4 . The structure simulation reveals that the RMSI can not only stabilize the PtSA on the electron-deficient g -C 3 N 4 via the strong chemical bond between PtSA and the two-coordinated C (C 2C ) sites caused by the N vacancies, but also promises the PtSA with an optimized electronic and geometric structures for capturing photogenerated electrons and producing H 2 . This finding opens a new channel for designing and manipulating single atom-loaded photocatalyst via the RMSI at a sub-zero low temperature.
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Scientific Reports
·
2019
·Vol. 9
·期 1
·1-14
·
IF 4.011
Wang Yizheng,Yu Jiang,Peng Weidong,Tian Jing,Yang Chun
In this paper, we used a facile ball milling, microwave radiation and heating treatment method to achieve the surface modification of TiO 2 with low g-C 3 N 4 concentration, and a multilayer heterojunction composite with TiO 2 as the main part and g-C 3 N 4 as the modification agent was obtained. The obtained materials were analyzed by several characterizations to get information on their chemical composition, crystalline structure, vibrational features and optical properties. The photocatalytic performance was evaluated by degradation of rhodamine B (RhB) and methylene blue (MB) under UV, visible and direct solar light irradiation. Its photocatalytic activity was enhanced depended on the novel structure of g-C 3 N 4 /TiO 2 hybrid and the special Z-scheme electron-hole transfer model of multilayer heterointerfaces. The material preparation and structural features could be useful for the design and development of other photocatalysts with high photocatalytic activity.
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CHEMICAL ENGINEERING JOURNAL
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2019
·
IF 8.355
Jianhua Zheng,Lei Zhang
In this study, a novel 3D magnetic Co 3 O 4 @CoO/g-C 3 N 4 ternary hybrid possessing double Z-scheme mechanism has been designed and architected by wet-impregnation and subsequent controlled oxidation process . In the Co 3 O 4 @CoO/g-C 3 N 4 ternary hybrid system, g-C 3 N 4 ultrathin nanopieces uniformly dispersed on each nanopetal of peony flower cobalt oxides , which not only helps to enhance the light absorption efficiency and avoid the aggregation but also readily promote the separation of photo-induced charge. Benefiting from the special hierarchical architecture, large open space between nanopetals and the synergistic effect between cobalt oxides and g-C 3 N 4 , when employed as photocatalyst for reduction of nitrobenzene (NB) and degradation of tetracycline (TC), 3D Co 3 O 4 @CoO/g-C 3 N 4 exhibited superior redox reactivity. Notably, a double Z-scheme heterojunctions and well matched band structures could further facilitate effective charge transfer. Meanwhile, Co 3 O 4 @CoO/g-C 3 N 4 ternary hybrids also exhibited excellent magnetic separation property and super cycling stability after four cycles, which make it a promising candidate as a visible light photocatalyst for practical application.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2019
·
IF 4.175
Xueding Jiang,Shufeng Lai,Weicheng Xu,Jianzhang Fang,Xin Chen,Jingzi Beiyuan,Xiwu Zhou,Kaichun Lin,Junxing Liu,Gongcou Guan
In this work, a novel visible-light-driven ternary BiOI/g-C 3 N 4 /CeO 2 photocatalyst was successfully synthesized by calcination and hydrothermal treatment . The obtained ternary BiOI/g-C 3 N 4 /CeO 2 had high photocatalytic performance for the degradation of tetracycline (TC) under visible-light irradiation. The samples were characterized by X-ray diffraction (XRD), UV–Vis diffuse reflectance (DRS) spectroscopy, and Fourier transform infrared spectroscopy (FT-IR), etc. The results indicated that 3 wt% BiOI/g-C 3 N 4 /CeO 2 catalyst possessed the best photocatalytic activity (91.6%) among all the as-prepared samples. The enhanced photocatalytic activity could be attributed to a double charge transfer process between g-C 3 N 4 and other catalysts in the ternary heterojunction , so that the separation of photogenerated electron–hole pairs was more effective. The as-prepared ternary sample also exhibited high stability after six cycles of the photodegradation reaction. Additionally, the active species (h + ) were considered as the main reactive species during the degradation of TC. Based on the research results, a possible photocatalytic reaction mechanism for the BiOI/g-C 3 N 4 /CeO 2 sample was proposed and discussed in detail.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2019
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IF 14.229
Yingying Jiao,Qunzeng Huang,Jianshe Wang,Zhanhang He,Zhongjun Li
A novel MoS 2 quantum dots (QDs) decorated g-C 3 N 4 nanosheet/N-doped carbon dots (NCDS) heterojunction photocatalyst was successfully synthesized by thermal polymerization and subsequent solvothermal approach. Under visible light (λ ≥ 420 nm) irradiation, the as-prepared g-C 3 N 4 /NCDS/MoS 2 composite with 3wt% of MoS 2 and 2wt% of NCDS displayed the highest photocatalytic hydrogen evolution activity with a corresponding H 2 evolution rate of 212.41μmol g −1 h −1 , which was about 53 times higher than that of g-C 3 N 4 /MoS 2 -3%. Moreover, the g-C 3 N 4 /NCDS/MoS 2 composite exhibited excellent photostability. The enhanced photocatalytic activity of g-C 3 N 4 /NCDS/MoS 2 composite was predominantly attributed to the formation of Z-scheme heterojunction between g-C 3 N 4 and NCDS, which effectively accelerated the transfer and separation of photogenerated charge carriers. Besides, the introduction of noble metal-free MoS 2 co-catalyst further promoted the separation of photogenerated charge carriers and provided more active sites for H 2 evolution reaction. The advantages of superior photocatalytic activity and excellent stability endowed a promising potential for g-C 3 N 4 /NCDS/MoS 2 composite to apply in photocatalytic fields.
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APPLIED SURFACE SCIENCE
·
2019
·
IF 5.155
Yangqing He,Zhengrui Huang,Zhanying Ma,Binghua Yao,Haiyang Liu,Linlin Hu,Qing Zhao,Qian Yang,Dongjie Liu,Deguo Du
In this study, zinc (II) 1, 8(11),15(18),22(25) - tetrakis (4-carboxylphenoxy) phthalocyanine (α-ZnTcPc) was synthesized as sensitizer to construct a novel photocatalyst α-ZnTcPc/g-C 3 N 4 by a polycondensation strategy. The FT-IR and XPS spectra demonstrated that the α-ZnTcPc molecules were covalently coupled on g-C 3 N 4 . The 10%α-ZnTcPc/g-C 3 N 4 composites exhibit excellent extended spectral response with intense broad near-infrared absorption at 695 nm and with significantly fascinated charge carrier separation. As expected, the 10%α-ZnTcPc/g-C 3 N 4 displayed a remarkable improved photocatalytic performance in decomposition of methylene blue (MB) and antibiotic tetracycline with degradation rates of 94.49% and 91.43% under visible light irradiation, respectively. The hydroxyl radicals (·OH) were observed as the main reactive oxidizing species in tetracycline decomposition. Moreover, the possible mechanism for enhanced visible light photocatalytic capability might be ascribed to the synergetic effect between α-ZnTcPc and g-C 3 N 4 , which creates large surface areas, decreases the recombination rate of photogenerated charge carries, as well as improves the visible light harvesting significantly. This work not only presents a practical method to conquer the drawback of pure g-C 3 N 4 , but also provides useful insights to construct other g-C 3 N 4 -based composites to take full advantage of solar light towards practical applications for eliminating recalcitrant organic pollutants.
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JOURNAL OF CATALYSIS
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2018
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IF 6.759
Zenan Hu,Junjie Zhou,Yongjian Ai,Lei Liu,Li Qi,Ruihang Jiang,Hongjie Bao,Jingting Wang,Jianshe Hu,Hong-bin Sun,Qionglin Liang
A magnetically separable 2D Rh/Fe 3 O 4 /g-C 3 N 4 -N catalyst has been synthesized for the catalytic transfer hydrogenation of nitroarenes to afford corresponding anilines. The highly dispersed Rh nanoparticles are the dominant active species. The reaction is second order for rhodium according to the kinetic study, and this means the activity of different Rh-containing catalyst can be precisely predicted and the active site contains two adjoining rhodium atoms. The strong interaction between Rh and Fe 3 O 4 contributes to the catalytic performance, therefore the obtained Rh/Fe 3 O 4 /g-C 3 N 4 -N catalyst exhibits excellent catalytic activity and chemoselectivity for the reduction of various nitroaromatics, and the turnover frequencies (TOF) can reach as high as 12,666 h −1 for 4-nitrophenol. Moreover, this catalytic system is environmentally friendly because of its green solvent water and harmless byproducts (H 2 O and N 2 ), and the catalyst shows outstanding stability and recyclability with at least 12 cycles.
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ACS Sustainable Chemistry & Engineering
·
2018
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IF 6.14
Binbin Shao,Zhifeng Liu,Guangming Zeng,Zhibin Wu,Yang Liu,Min Cheng,Ming Chen,Yujie Liu,Wei Zhang,Haopeng Feng
Herein, the nitrogen-doped hollow mesoporous carbon spheres (N-HMCs) modified g-C3N4/Bi2O3 direct dual semiconductor photocatalyst (g-C3N4/Bi2O3@N-HMCs) were synthesized by a facile thermal process. The morphology, structure, elements, and photoelectrochemical properties of the as-prepared samples were characterized by electron microscopy, N2 sorption–desorption, X-ray diffraction, X-ray photoelectron spectroscopy, diffuse-reflectance spectra, and photoluminescence spectroscopy, among other technologies. The photocatalytic efficiency was evaluated toward degradation of antibiotics tetracycline hydrochloride (TCH) and ciprofloxacin hydrochloride (CFH) under visible-light irradiation, and the results showed that the g-C3N4/Bi2O3@N-HMCs composite exhibited superior photocatalytic efficiency than other comparison samples, which could be attributed to the synergistic action of g-C3N4/Bi2O3 direct dual semiconductor photocatalytic system and the N-HMCs. The characterization techniques revealed that N-HMCs play three vital roles in improving photocatalytic efficiency. First, N-HMCs could serve as a photosensitizer to enhance visible-light absorption. Second, N-HMCs are an excellent conductive material to transfer the photoexcited electrons quickly to hinder the electron–hole pairs recombination. Third, N-HMCs could provide more active sites in the photocatalytic process. The scavenger experiments and electron-spin-resonance results revealed that the active substances h+, •O2–, and •OH performed together in the photodegradation system. Additionally, the g-C3N4/Bi2O3@N-HMCs composite showed favorable photostability after six rounds of recycling, suggesting the great prospects of the practical application of g-C3N4/Bi2O3@N-HMCs.
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Small
·
2018
·Vol. 14
·期 33
·1801812
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IF 9.598
Kai Gu,Xueting Pan,Weiwei Wang,Junjie Ma,Yun Sun,Hailong Yang,Heyun Shen,Zhijun Huang,Huiyu Liu
Loading novel metal nanosheets onto nanosheet support can improve their catalytic performance, but the morphological incompatibility makes it difficult to construct a well-contacted interface, which is of particular interest in supported catalysts. Herein, Pd nanosheets (Pd NSs) are supported onto graphitic carbon nitride nanosheets (CNNSs) with intimate face-to-face contact through an in situ growth method. This method overcomes the limitations of the morphological incompatibility and ensures the intimate interfacial contact between Pd NSs and CNNSs. The nitrogen-rich nature of CNNSs endows Pd NSs with abundant anchoring sites, which optimizes the electronic structure and improves the chemical and morphological stability of Pd NSs. The supported Pd NSs demonstrate high dispersion and exhibit largely enhanced activity toward the reduction of 4-nitrophenol. The concentration-normalized rate constant is up to 3052 min −1 g −1 L, which is 5.4 times higher than that obtained by unsupported Pd NSs. No obvious deactivation is observed after six runs of the recycling experiments. It is believed that the supported novel metal nanosheets with the intimately contacted interface may show promising applications in catalysis.
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Inorganic Chemistry Frontiers
·
2017
·Vol. 5
·期 2
·481-489
·
IF 4.036
Wanbao Wu,Xu Li,Zhaohui Ruan,Yudong Li,Xianzhu Xu,Yuan Yuan,Kaifeng Lin
A TiO2 trapped meso/macroporous g-C3N4 heterojunction (mm-CNT) photocatalyst is fabricated by hydrolysis and sintering of tetrabutyl titanate on meso/macroporous g-C3N4 prepared via a facile hard template method. TiO2 nanoparticles are highly dispersed and some of them are trapped in the pores of meso/macroporous g-C3N4. The photocatalytic performance of mm-CNT is assessed through degradation of Rhodamine B solution under visible light irradiation, which displays much better photocatalytic performance than that over pristine meso/macroporous g-C3N4 and pristine g-C3N4. Based on the characterization results, it is reasonable to believe that the enhanced photocatalytic activity should be attributed to the unique meso/macroporous architecture and heterojunction structure, which results in improved mass transfer and enhances the separation efficiency of exciton dissociation. Besides, an optical simulation is initially utilized to study the optical absorption characteristics of mm-CNT since the optical absorption ability of a photocatalyst is one of the most important aspects influencing the photocatalytic ability. As a result, the enhanced ability of light absorption observed on the heterojunctions should be also favorable to achieve improved photocatalytic performances. On account of the analysis results, a possible photocatalytic mechanism for enhanced visible light photocatalytic activity is proposed.
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CHEMICAL ENGINEERING JOURNAL
·
2017
·
IF 6.216
Zhi Zhu,Pengwei Huo,Ziyang Lu,Yongsheng Yan,Zhi Liu,Weidong Shi,Chunxiang Li,Hongjun Dong
A novel efficient magnetic oxidation-reduction like-Z-scheme structure photocatalyst composed of g-C 3 N 4 , CdS and the oxidation-reduction mediators of Fe 3 O 4 is successfully synthesized by heat treatment methods. The like-Z-scheme CdS/Fe 3 O 4 /g-C 3 N 4 photocatalyst exhibits universal degradation property on removing kinds of antibiotics, and the photocatalytic activity is better than that of CdS/g-C 3 N 4 and pure g-C 3 N 4 . The excellent photocatalytic performance is originated from the unique like-Z-scheme structure and oxidation–reduction function of Fe 3 O 4 , which effectively separates the hole-electron and sufficiently utilizes the photogenerated carriers for generating more active radicals. The results showed that when the content of Fe 3 O 4 is 10%, the CdS/Fe 3 O 4 /g-C 3 N 4 exhibited superior activity. The best degradation rate constant K in the like-Z-scheme photocatalyst is approximately 26 times of pure g-C 3 N 4 . The important role of Fe 3 O 4 and the photocatalytic mechanism are also discussed in detail. This work not only puts forward a novel design idea of the like-Z-scheme material, but also is expected to be widely applied to the universal removal of kinds of antibiotics according to the practical requirement.
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MICROCHEMICAL JOURNAL
·
2024
·
IF 4.9
Hong Zhang,Zhigao Zhang,Longyang Han,Mingqin Zhao,Pengfei Liu,Zhen Luo
Aflatoxin B 1 (AFB 1 ) has seriously threatened human health, so it is vital to construct an efficient detection strategy for AFB 1 analysis. An exquisitely designed ratiometric electrochemical aptasensor for sensitive detection of AFB 1 has been successfully developed in this work. DNA tetrahedral scaffold (DTS) is used to fix the DNA probes, 3D DNAzyme walker is employed to amplify the detection signals, and the composite material AuNP/ZIF-67/g-C 3 N 4 acts as the sensing surface of the detection electrode. In the presence of AFB 1 , the 3D DNAzyme walker induced the release of the oligonucleotide attached ferrocene (Fc) from the detection electrode and is simultaneously grafted the DNA-modified methylene blue (MB) onto the electrode, leading to a seesaw-like ratiometric electrochemical aptasensor. This ratiometric electrochemical aptasensor provides an outstanding AFB 1 analysis in the linear range of 2.0 fg·mL −1 to 1.0 ng·mL −1 with the limit of detection (LOD) 0.67 fg·mL −1 . It provides new idea for the analysis of other contaminants in foodstuffs.
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