Catalysts
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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
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RSC Advances
·
2023
·Vol. 13
·期 13
·8915-8922
·
IF 3.9
Tong Zhou,Haitang Wei,Bin Xiao,Tianping Lv,Liangfei Duan,Qingjie Lu,Jin Zhang,Yumin Zhang,Qingju Liu
One of the most promising strategies for producing hydrogen is photocatalytic water splitting, in which the photocatalyst is a key component. Among many semiconductor photocatalysts, g-C3N4 has attracted great attention due to its narrow band gap, excellent stability and low cost. However, practical application is limited by its poor intrinsic activity. In this work, a high-performance porous g-C3N4 (PCN) photocatalyst with anchored Cu single atoms (CuSAs) was synthesized by a one-step co-heating approach. The obtained Cu1.5–PCN displays an excellent hydrogen evolution rate (HER) of 2142.4 μmol h−1 g−1 under visible light (=420 nm), which is around 15 and 109 times higher than those of PCN and bulk g-C3N4, respectively. In addition, it also shows good stability during H2 evolution. The results of experimental research and DFT simulations indicate that the single Cu ions formed bonds with the N-ring and these remain stable. Meanwhile, the special electronic structure of the Cu–N charge bridge extends the light absorption band to the visible-light region (380–700 nm). This high-performance and low-cost photocatalyst has great potential in solar energy conversion.
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PubMed
高影响因子
RSC Advances
·
2023
·Vol. 13
·期 10
·6442-6452
·
IF 3.9
Jinlong Wang,Hao Song,Peipei Dong,Zihan Zhao,Yanjie Zhang
Nowadays, considerable efforts have been extensively devoted to explore a general strategy for improving the color uniformity and thermal stability of phosphors, which is vital for its applications in health and comfort lighting. In this study, the SrSi2O2N2:Eu2+/g-C3N4 composites were successfully prepared via a facile and effective solid-state method to improve their photoluminescence properties and thermal stability. The coupling microstructure and chemical composition of the composites were demonstrated by high-resolution transmission electron microscopy (HRTEM) and EDS line-scanning analyses. Notably, the dual emissions at ∼460 nm (blue) and ∼520 nm (green) were observed for the SrSi2O2N2:Eu2+/g-C3N4 composite under near-ultraviolet (NUV) excitation, attributed to the g-C3N4 and 5d–4f transition of Eu2+ ions, respectively. The coupling structure will be beneficial to the color uniformity of the blue/green emitting light. Further, SrSi2O2N2:Eu2+/g-C3N4 composites exhibited a similar photoluminescence intensity compared with the SrSi2O2N2:Eu2+ phosphor even after thermal treatment at 500 °C for 2 h due to the protection of g-C3N4. The decreased decay time (1798.3 ns) of green emission for SSON/CN compared with SSON phosphor (1835.5 ns) indicated that the coupling structure suppressed the non-radiative transition and improved photoluminescence properties and thermal stability. This work provides a facile strategy to construct SrSi2O2N2:Eu2+/g-C3N4 composites with coupling structure for improved color uniformity and thermal stability.
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MATERIALS CHEMISTRY AND PHYSICS
·
2019
·
IF 2.781
Jirong Bai,Haiyang Xu,Gang Chen,Wenhua Lv,Zhijiang Ni,Zhilei Wang,Jiaying Yang,Hengfei Qin,Zheng Zheng,Xi Li
α-Fe 2 O 3 /porous g-C 3 N 4 (α-Fe 2 O 3 /PCN) photocatalysts were fabricated via a facile and green method. Structural characterization indicated α-Fe 2 O 3 nanoparticles were successfully loaded onto PCN. The α-Fe 2 O 3 /PCN nanocomposites were proven durable with significantly enhanced photocatalytic activity for Rhodamine B photodegradation than the single components under visible light irradiation. The improved photoactivity was mainly attributed to the broadened visible light absorption, enriched active sites, and formation of α-Fe 2 O 3 /PCN heterojunction that addressed the recombination of photoinduced electrons and holes. The α-Fe 2 O 3 /PCN hybrids also showed high recyclability and chemical stability.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2019
·
IF 14.229
Ruiyang Zhang,Penghui Li,Fang Wang,Liqun Ye,Abhijeet Gaur,Zeai Huang,Ziyan Zhao,Yang Bai,Ying Zhou
Atomically dispersed atom catalysts with atomically distributed active metal centers have attracted great attention owing to the maximum atom efficiency and excellent selectivity. Herein, for the first time, we found atomically dispersed Mo atoms can be formed on g-C 3 N 4 , and induce its amorphous transformation. This amorphous transformation leads to the formation of strong band tails with remarkably enhancing the absorbance edge of Mo-C 3 N 4 up to 750 nm, resulting in almost whole visible-light range absorption. The formation of new Mo-C and Mo-N bonds due to strong interfacial interaction between atomically dispersed Mo atoms and g-C 3 N 4 provide new electron and hole transport pathways to accelerate the separation of charge carriers. As a result, amorphous Mo/C 3 N 4 (a-Mo/C 3 N 4 ) reveals excellent photoreduction of CO 2 , yielding CO and H 2 productions of 18 and 37 μmol g −1 h −1 under visible-light illumination (λ > 420 nm), which manifest a remarkable 10.6- and 4-folds enhancement of that over crystalline g-C 3 N 4 . This finding provides a conceptually different approach to fabricate high-efficient photocatalyst through the strong interfacial interaction between atomically dispersed metal atoms and host.
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MATERIALS CHEMISTRY AND PHYSICS
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2018
·
IF 2.21
Hongduo Yao,Xiaoxue Wang,Jianping Gao,Chunjuan Gao,Ruiru Zhao,Xiangang Zhai,Yongli Wu,Chaoyue Hao,Jiangbing Yang,Shunkang Mei,Haixia Qiu
Waste water treatment with adsorbents has become one of the most effective methods. In this work, we have reported the preparation of the flower-like Cu 2 MoS 4 /g-C 3 N 4 composites. The Cu 2 MoS 4 nanosheets were arranged in a flower-like structure by a simple one-step hydrothermal synthesis method and attached to g-C 3 N 4 nanosheets. The as-prepared flower-like Cu 2 MoS 4 /g-C 3 N 4 composites was found to have potential for the adsorption of RhB in aqueous solution. The microstructure of the product was analyzed by X-ray diffraction (XRD), Fourier transform infrared (FT-IR) spectra, X-ray photoelectron spectroscope (XPS), transmission electron microscopy (TEM), energy dispersive spectroscopy (EDS), scanning electron microscopy (SEM) and Brunauer-Emmett-Teller (BET). The effects of the ratio of the composite material, the initial concentration of the dye and the contact time were explored. The Langmuir maximum adsorption capacity of the flower-like Cu 2 MoS 4 /g-C 3 N 4 composites for RhB was reached 420.2 mg/g. Moreover, the adsorption process is consistent with the pseudo second-order kinetic model, the Langmuir isotherms model and the Freundlich isotherms model.
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Catalysis Science & Technology
·
2019
·Vol. 9
·期 10
·2571-2577
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IF 5.726
Weiliang Qi,Siqi Liu,Fei Li,Heng Jiang,Zhixing Cheng,Shanlin Zhao,Minghui Yang
Transition metal nitrides have been recognized as excellent hydrogen evolution electrocatalysts and therefore are promising alternative co-catalysts for photocatalytic hydrogen production. Herein, iron nitride (Fe2N) nanoparticles have been prepared by using MOFs as sacrificial precursors. A novel g-C3N4–Fe2N nanostructure has been fabricated by an electrostatic self-assembly method at room temperature for photocatalytic H2 evolution. MOF-derived Fe2N nanoparticles as co-catalysts can promote photo-generated charge-carrier transportation/separation and decrease the overpotential of H2-evolution. Therefore, the optimal g-C3N4–Fe2N nanocomposite exhibits an obviously improved H2 evolution rate of 88.7 μmol g−1 h−1, which is almost 48 times higher than that of pure g-C3N4 nanosheets.
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APPLIED ORGANOMETALLIC CHEMISTRY
·
2018
·Vol. 33
·期 3
·e4683
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IF 3.581
Jiang Li,Xiaolu Zhu,Fengxian Qiu,Tao Zhang,Fengping Hu,Xiaoming Peng
Introducing plasmonic metals into semiconductor materials has been proven to be an attractive strategy for enhancing photocatalytic activity in the visible region. In this work, a novel and efficient Ag/Ag 2 WO 4 /g-C 3 N 4 (AACN) ternary plasmonic photocatalyst was successfully synthesized using a facile one-step in situ hydrothermal method. The composition, structure, morphology and optical absorption properties of AACN were investigated using X-ray diffraction, Fourier transform infrared spectroscopy, scanning electron microscopy, and UV–visible diffuse reflectance spectroscopy, respectively. Photocatalytic performance of AACN was evaluated via rhodamine B and tetracycline degradation. The results indicated that AACN had excellent photocatalytic performance for rhodamine B degradation with a rate constant of 0.0125 min −1 , which was higher than those of Ag 2 WO 4 and Ag/Ag 2 WO 4 . Characterization and photocatalytic tests showed that the strong coupling effect between the Ag/Ag 2 WO 4 nanoparticles and the exfoliated ultrathin g-C 3 N 4 nanosheets was superior for visible-light responsivity and reduced the recombination rate of photogenerated electrons and holes. A proposed mechanism is also discussed according to the band energy structure and the experimental results.
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SENSORS AND ACTUATORS B-CHEMICAL
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2018
·
IF 5.667
Tianrong Zhan,Xia Tian,Guiyan Ding,Xien Liu,Lei Wang,Hongni Teng
We have developed a facile quaternarization strategy to an ultrathin lamellar g-C 3 N 4 ionic liquid nanostructure (IL-CNNS) via a nucleophilic substitution between the tertiary amino groups in tri- s -triazine subunits and n-butyl bromide. After functionalization, the obtained IL-CNNS composite exhibits the enhanced conductivity, dispersibility and stability owing to the formation of IL structure. This composite has been characterized by several spectroscopic techniques (FT-IR, XRD, XPS, TGA and TEM). The IL-CNNS modified electrode displays the larger effective surface area and the faster electron transfer rate, hence resulting in the superior electrocatalytic activity toward 2,4-Dichlorophenol (2,4-DCP). Under the optimal conditions, the proposed 2,4-DCP sensor gives rise to the wide linear range from 0.02 to 160 μM with a low detection limit (6.21 nM, S/N = 3) by amperometric method. The developed sensor has been applied to detect 2,4-DCP in water samples with satisfactory recoveries and stability. This quaternarization strategy may open up a new avenue to fabricate the layered carbon nitride IL nanostructure for electrochemical sensing applications.
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APPLIED SURFACE SCIENCE
·
2019
·
IF 5.155
Yao Chen,Fei Ding,Aung Khaing,Dong Yang,Zhongyi Jiang
Graphic carbon nitride (g-C 3 N 4 ) is a kind of promising organic semiconductor in visible light driven photocatalysis due to its metal free, high physicochemical stability and appealing electronic band structure . In this work, a porous hexagonal-prism g-C 3 N 4 (ACNH) photocatalyst was successfully synthesized via an acetic acid-assisted supramolecular assembly approach followed by calcination . The resulting ACNH materials have a corrugated and closely packed porous structure, which is composed of thin layers about 30 nm in thickness. The specific surface area of ACNH is as high as 67.7 m 2 g −1 , which is approximately 8-fold of bulk g-C 3 N 4 . Moreover, the porous structure induces the red shift of the absorption edge and facilitates the photo-induced charge separation of g-C 3 N 4 . Compared to bulk g-C 3 N 4 , the ACNH sample exhibits almost 13-fold improvement for the RhB degradation with the rate constant of 0.053 min −1 . This finding suggests that the acid-assisted supramolecular assembly may become a feasible method to synthesize g-C 3 N 4 -based photocatalysts with higher surface area and photocatalytic activity .
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2019
·
IF 5.107
Changlin Yu,Hongbo He,Wanqin Zhou,Zhen Liu,Longfu Wei
An interesting rugby-ball-like Zn 3 (PO 4 ) 2 @C 3 N 4 photocatalyst with well- controlled structures as high-efficient visible-light photocatalysts was synthesized via two steps of solvothermal-grinding calcination method. The composition, structure, morphology, and optical absorption properties of as-synthesized Zn 3 (PO 4 ) 2 @C 3 N 4 samples were intensively characterized by XRD, N 2 physical adsorption, SEM, TEM, FT-IR, UV–vis DRS, XPS, PL and photoelectrochemical measurements, respectively. The formation of C 3 N 4 shell obviously increased the surface area and induced the rich pore structures. The intimate interface between Zn 3 (PO 4 ) 2 and C 3 N 4 phase obviously enhanced the transport rate of photogenerated carriers and restrained the recombination of photogenerated electrons and holes. The optimal Zn 3 (PO 4 ) 2 @C 3 N 4 (35 wt%) exhibited the highest adsorption and photocatalytic activity in the degradation of methylene blue (MB), which was 150 and 7.5 times as high as C 3 N 4 , respectively. Moreover, the robust Zn 3 (PO 4 ) 2 @C 3 N 4 nanoheterojunctions fabricated by this grinding-calcination route have high stability in recycling reactions.
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JOURNAL OF THE AMERICAN CERAMIC SOCIETY
·
2019
·Vol. 102
·期 11
·6517-6528
·
IF 3.094
Liu Pei,Yan Xu,Jiaqiang Liu,Junbiao Wu,Yide Han,Xia Zhang
Morphology modulation of photocatalyst has been demonstrated to be a crucial strategy for improving the catalytic performance in solar energy conversion system. Here we systematically investigated the influence of the solvent-dependent morphology evolution of Zn 2 GeO 4 phase on the photocatalytic efficiency of the as-prepared g-C 3 N 4 /Zn 2 GeO 4 composites. The morphologies of Zn 2 GeO 4 were rationally tuned from flower-like nanosheets to length-controllable nanorods, and microclusters assembled from microrods through regulating the solution polarity of different organic solvents. Accordingly, the Zn 2 GeO 4 sample prepared in ethylene glycol (EG) with long rod-like morphology and integrated with g-C 3 N 4 , abbreviated as g-C 3 N 4 /Zn 2 GeO 4 (1:1)-EG, exhibited the best visible-light absorption ability and the highest efficiency. The synergetic effect of the long rod-like Zn 2 GeO 4 phase with many exposed (110) crystalline facets and g-C 3 N 4 accelerates the separation and interface transportation of photoexcited charge carriers, as confirmed by photocurrent measurements. The MB degradation mechanism was also proposed to clarify the charge-transfer process and the improved photodegradation activity. This study offers an experimental basis for understanding the significance of morphology control on rational design of photocatalysts with improved performance.
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