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Nanoscale Advances · 2020 ·Vol. 2 ·期 11 ·5396-5402 · IF 0

The dual interfacial modification of 2D g-C3N4 for high-efficiency and stable planar perovskite solar cells

Zhou Liu,Shuzhen Wu,Xiaojie Yang,Yijun Zhou,Jiaren Jin,Junmei Sun,Li Zhao,Shimin Wang

Carrier recombination and charge loss at the interfaces of perovskite layers have a significant influence on high-performance planar perovskite solar cells (PSCs). We employed two-dimensional graphitic carbon nitride (g-C3N4), which is a heat-resistant n-type semiconductor, to modify the electron-transport layer/perovskite and perovskite/hole-transport layer interfaces, respectively. g-C3N4 could passivate the surface trap states of the methylammonium lead iodide light absorber through the formation of a Lewis adduct between N and the under-coordinated Pb, and it could also remarkably reduce the grain boundaries between perovskite crystal particles. A maximum power conversion efficiency (PCE) of 19.67% (Voc = 1.14 V, Jsc = 21.45 mA cm−2, FF = 0.807) could be obtained from planar PSCs with long-term stability using dual-positioned g-C3N4. Therefore, we consider that ultrathin semiconductor films with a Lewis base nature are suitable as dual-functional transport materials for devices. This work provides new guidance for dual-interfacial modification to improve the PCE and stability of devices.

研究领域: 材料科学 · 新能源 · 半导体器件 · 界面工程 · 光电子学
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2019 · IF 6.361

Yeast-derived carbon sphere as a bridge of charge carriers towards to enhanced photocatalytic activity of 2D/2D Cu2WS4/g-C3N4 heterojunction

Huinan Che,Guangbo Che,Pengjie Zhou,Chunbo Liu,Hongjun Dong

It is very challenging to fabricate novel, high-efficiency photocatalysts with an enhanced visible light absorption capacity, high charge carrier separation efficiency, and large specific surface area . For this purpose, a yeast-derived carbon (YC) sphere was added as a charge carrier bridge to the 2D-2D Cu 2 WS 4 /g-C 3 N 4 heterojunction through a facile hydrothermal method . The YC sphere, as a bridge for electrons, is not only advantageous in inhibiting rapid recombination by electrons, but also remarkably enhances the visible light absorption capacity. Moreover, the YC sphere can also increase the specific surface area and surface roughness , which can enhance the adsorption of pollutant molecules and provide abundant active sites for photocatalytic reactions. The g-C 3 N 4 /YC/Cu 2 WS 4 heterojunction showed the best photocatalytic activity for reducing hexavalent chromium Cr(VI) and decomposing tetracycline (TC) under visible light. Meanwhile, the acute toxicity of Daphnia magna (D. magna) gradually decreases with the conversion of Cr(VI) to Cr(III) in solution. In addition, the possible intermediate products and the photocatalytic reaction mechanism are revealed in depth. This work provides a general example for improving the photocatalytic activity of 2D-2D based heterojunctions by introducing a biomass material.

研究领域: 材料科学 · 环境科学
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JOURNAL OF NANOSCIENCE AND NANOTECHNOLOGY · 2020 ·Vol. 20 ·期 12 ·7469-7479 · IF 1.134

Magnetic Solid-Phase Extraction Based on Fe3O4/g-C3N4 Nanocomposite for the Determination of Polychlorinated Biphenyls and Polychlorinated Diphenyl Ethers in Environmental Waters

Ji Dongliang,Zhang Meixing,Geng Xinxiang,Zha Zhenxing,Li Ying,Yang Jing,Cui Shihai

The graphitic carbon nitride (g-C3N4) and the Fe3O4/g-C3N4 magnetic materials were synthesized in this paper. The structures of the materials were confirmed by a series of analysis. The Fe3O4/g-C3N4 was then used as a sorbent to adsorb polychlorinated diphenyl ethers and polychlorinated biphenyls. Different extraction conditions were examined, including adsorbent amount, salinity, pH of the sample matrix, adsorption time, reaction temperature, elution solvent and preconcentration factor. The maximum recoveries were obtained by employing methanol to desorb pollutants on 40.0 mg Fe3O4/g-C3N4 in 120.0 mL environmental water with a salinity of 5% (w/v) at a pH of 7 at 25 °C within 10 min. Using the optimized parameters, the detection limits of the method are between 0.01 and 0.04 μ · L−1 with a satisfying linear relationship. The adsorbent can be recycled at least 10 times with no significant reduction in the extraction efficiency.

研究领域: 分析化学 · 环境科学
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Journal of Inorganic and Organometallic Polymers and Materials · 2021 ·Vol. 32 ·期 3 ·973-983 · IF 3.543

Photocatalytic Degradation of Composites with Magnesium Aluminum Hydrotalcite Derived Metal Oxides and g-C3N4

Yu Mingwei,Zhang Lianhong,Wen Jie,Zhang Hui,Liu Faping,Lv Yanjun,Zhao Xiaodong

The remove of the organic pollutants in water plays an important role on the environmental protection, thus photocatalysis, as an effective method, has been attained much attention to deal with this problem. In this paper, a composite of g-C 3 N 4 and Mg–Al hydrotalcite derived metal oxides was prepared by simple co-precipitation methods followed by calcination. The effective adsorption-photocatalysis synergic effect and highly efficient removal of organic pollutants from water under simulated sunlight irradiation was found in the presence of fabricated metal oxide nanocomposites. The photocatalytic degradation rate of methylene blue reached 97.3% within 1 h under visible light, and the degradation rate constant was 0.0432 min −1 , which is 3.6 times that of g-C 3 N 4 . Though characterization analysis, more active sites are exposed to absorb more organic pollutants on the mater surface in the presence of the open hierarchical structures of composite materials, and the "face to face" contact structure between 2D materials is formed to promote the separation of electrons and holes. The photocatalytic degradation was stable in the recycling process of the catalyst. In addition, the photocatalytic degradation mechanism of the catalyst was explained by free radical scavenging experiment. The material provides an effective method for removing organic pollutants in water, and has broad application prospects.

研究领域: 环境科学 · 材料科学 · 化学工程 · 水处理
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CHEMICAL ENGINEERING JOURNAL · 2020 · IF 10.652

Construction of a visible-light-driven magnetic dual Z-scheme BiVO4/g-C3N4/NiFe2O4 photocatalyst for effective removal of ofloxacin: Mechanisms and degradation pathway

Guanshu Zhao,Jing Ding,Fanyang Zhou,Xueqi Chen,Liangliang Wei,Qingwei Gao,Kun Wang,Qingliang Zhao

Inefficient utilization of photo-induced charge carriers and low recyclability are limitations for photocatalyst to get access to the practical application. A novel ternary BiVO 4 /g-C 3 N 4 /NiFe 2 O 4 composite with dual Z-scheme heterojunction was successfully developed and constructed to enhance the separation of photo-induced charge carriers and the absorption range of visible light. The structure, composition, morphology, magnetic, and optical properties of this photocatalyst were investigated comprehensively. The photocatalytic performance, mechanism, and pathway of ofloxacin degradation under visible light were studied. Results indicated that the internal interaction between different semiconductors presented the successful fabrication of ternary composite, and its red shift of adsorption range of visible light contributed to an enhancement of photocatalytic ability. The as-prepared ternary composite exhibited highest photocatalytic removal rate constant for ofloxacin, which was 3.8, 16.3 and 71.2 times as much as that of the pure BiVO 4 , pure g-C 3 N 4 and pure NiFe 2 O 4 , respectively. The five successive recycling experiments exhibited the high photocatalytic stability of the as-prepared catalyst, with simple recovery operation due to its magnetic property. The holes and superoxide radicals dominated the photocatalytic degradation process of pollutants. A dual Z-scheme heterojunction other than conventional heterojunction was responsible for the enhancement on redox capacity and the separation of charge carriers. Different transformation products during ofloxacin photocatalytic degradation were identified and transformation pathway was put forward. This study provides a promising strategy on the application of visible-light-driven photocatalysts in water treatment.

研究领域: 环境科学 · 材料科学
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Journal of Materials Chemistry A · 2019 ·Vol. 7 ·期 12 ·6939-6945 · IF 10.733

Modulating charge transfer dynamics for g-C3N4 through a dimension and interface engineered transition metal phosphide co-catalyst for efficient visible-light photocatalytic hydrogen generation

Fu Zhang,Jihua Zhang,Jianming Li,Xu Jin,Yapeng Li,Min Wu,Xiongwu Kang,Tao Hu,Xiaoqi Wang,Wei Ren,Genqiang Zhang

Transition metal phosphide (TMP) co-catalysts have been widely applied to modify graphitic carbon nitride (g-C3N4) for improving the photocatalytic activity, but it is still a great challenge to fabricate high performance and stable g-C3N4 based photocatalysts decorated with TMP co-catalysts by simple approaches. Herein, we report a facile and general strategy for the synthesis of TMP/g-C3N4 hybrid photocatalysts with high H2 production performance under visible light irradiation. Among the as-prepared TMP/g-C3N4 hybrids, the CoP/g-C3N4 sample with an optimum mass content of 2.5 wt% delivers the highest photocatalytic H2 evolution rate of 956.8 μmol g−1 h−1. DFT calculations and experimental results reveal that the superior catalytic activity could be predominantly attributed to the larger number of active sites and the enhanced photo-excited charge transfer dynamics benefitting from the synergistic effect of the ultrasmall particle size and the intimate contact interface between g-C3N4 and CoP. We anticipate that the protocol would provide a promising strategy for designing TMP co-catalyst based hybrid nanostructures aiming to optimize photocatalytic hydrogen generation efficiency.

研究领域: 材料科学 · 催化化学 · 能源科学
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MATERIALS SCIENCE IN SEMICONDUCTOR PROCESSING · 2020 · IF 3.085

Visible-light-responsive K-doped g-C3N4/BiOBr hybrid photocatalyst with highly efficient degradation of Rhodamine B and tetracycline

Junnan Qu,Yi Du,Yibing Feng,Jianyong Wang,Bo He,Minxing Du,Yang Liu,Nan Jiang

A visible-light-responsive hybrid photocatalyst , K-doped g-C 3 N 4 /BiOBr, has been synthesized by K-doped g-C 3 N 4 (K–CN) and BiOBr. The property of photocatalysts was characterized by XRD , FT-IR, TEM, SEM , DRS , PL , EIS and HPLC. The photocatalytic activity of K-doped g-C 3 N 4 /BiOBr was evaluated by degradation of Rhodamine B (RhB) and tetracycline hydrochloride under visible-light irradiation. The K-doped g-C 3 N 4 /BiOBr hybrid photocatalyst which contains K–CN with mass fraction of 20% (20K–CN/BiOBr) shows the best degradation efficiency of RhB. The degradation efficiency of RhB (20 mg/L) can be achieved to 99% and the degradation efficiency of tetracycline hydrochloride by BiOBr decreased with the increase of K-doped g-C 3 N 4 doping. The results of photocurrent and EIS assumed that the tight coupling between K–CN and BiOBr can enhance the separating efficiency of photo-generated carrier. In addition, the capture experiment proof that h + is the primary active substance in the system of reaction and ·OH is the auxiliary active substance. After five degradation experiments, the efficiency of the degradation of Rhodamine B by the sample can still reach 90%, which proves that the samples are stable. A new and efficient method is provided in this work to solve the pollution of organic dyes and antibiotics.

研究领域: 环境科学 · 材料科学
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JOURNAL OF ALLOYS AND COMPOUNDS · 2022 · IF 6.371

Heteroatom bay-annulated perylene imides/g-C3N4 heterojunctions for efficient photocatalytic H2O2 evolution

Shufan Feng,Yan-Ping Zhang,Huihui Xu,Xue-qing Gong,Jianli Hua

Developing environmental-friendly photocatalysts with efficient photocatalytic activity is a promising way to tackle energy and environment issues. In this paper, perylene diimide (PDI) and its four derivatives ( SF-HPDI , N-HPDI , S-HPDI, and Se-HPDI ) with variable substituents at the bay position were synthesized and further used to construct the heterojunctions with g-C 3 N 4 for photocatalytic H 2 O 2 evolution. Among them, Se-HPDI /g-C 3 N 4 heterojunction achieves the highest H 2 O 2 production rate of 224.27 μM h –1 under visible light, which is 10.1 times higher than that of bare g-C 3 N 4 . The enhancement is because introducing substituents at the bay position increases the disparity of electron distribution between different constituent layers in heterojunctions, which is conducive to improving the interfacial electric field. Also, the load of PDIs broadens the optical absorption range of g-C 3 N 4 and suppresses H 2 O 2 decomposition. This work may inspire the further design of PDI-based photocatalysts.

研究领域: 材料科学 · 环境科学 · 光化学 · 催化
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APPLIED CATALYSIS B-ENVIRONMENTAL · 2014 · IF 6.007

Study on the separation mechanisms of photogenerated electrons and holes for composite photocatalysts g-C3N4-WO3

Shifu Chen,Yingfei Hu,Sugang Meng,Xianliang Fu

The separation mechanisms of photogenerated electrons and holes for composite photocatalysts have been a research focus. In this paper, the composite g-C 3 N 4 -WO 3 photocatalysts with different main parts of C 3 N 4 or WO 3 were prepared by ball milling and heat treatment methods. The photocatalytic performance was evaluated by degradation of methylene blue (MB) and fuchsin (BF) under visible light illumination. The photocatalyst was characterized by X-ray powder diffraction (XRD), UV–vis diffuse reflection spectroscopy (DRS), transmission electron microscopy (TEM) and Brunauer–Emmett–Teller (BET) methods. The separation mechanisms of photogenerated electrons and holes of the g-C 3 N 4 -WO 3 photocatalysts were investigated by electron spin resonance technology (ESR), photoluminescence technique (PL), and determination of reactive species in the photocatalytic reactions. When the main part of the g-C 3 N 4 -WO 3 photocatalyst is WO 3 (namely g-C 3 N 4 /WO 3 ), the transport process of the photogenerated electrons and holes adopts the generic band–band transfer. Meanwhile, g-C 3 N 4 is covered by WO 3 powder, and the role of g-C 3 N 4 can not be played fully. The photocatalytic activity of the photocatalyst is not obviously increased. However, when the primary part of the WO 3 -g-C 3 N 4 photocatalyst is g-C 3 N 4 (namely WO 3 /g-C 3 N 4 ), the migration of photogenerated electrons and holes exhibits a typical characteristic of Z-scheme photocatalyst, and the photocatalytic activity of the photocatalyst is increased greatly.

研究领域: 材料科学 · 环境科学 · 光催化技术
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ACS Applied Materials & Interfaces · 2020 · IF 8.758

Construction of the 1D Covalent Organic Framework/2D g-C3N4 Heterojunction with High Apparent Quantum Efficiency at 500 nm

Yanmei Xing,Liying Yin,Yingnan Zhao,Zhilu Du,Hua-Qiao Tan,Xing Qin,Wingkei Ho,Tianyu Qiu,Yang-Guang Li

The reasonable construction of heterojunction photocatalysts with clear nanostructures and a good interface contact especially the one-dimensional/two-dimensional (1D/2D) composite heterojunction with unique morphology is considered one of the most effective strategies for designing highly efficient photocatalysts. Herein, a series of the 1D β-keto-enamine-based covalent organic framework (COF)/2D g-C3N4 composite materials COF–CN (1:x; where 1:x represents the mass ratio of COF and g-C3N4, x = 2.5, 5, 10, 15, 20) is prepared through the in situ reaction of 2,4,6-triformylphloroglucinol (Tp) and benzidine (BD) in stripped g-C3N4 suspension. A series of characterizations, such as X-ray diffraction (XRD), Fourier transform infrared (FT-IR), scanning electron microscopy (SEM), and transmission electron microscopy (TEM), have verified their 1D/2D heterojunction structure. With the introduction of 1D COF nanobelts, the absorption of the composite is largely extended to 560 nm. Photocatalytic experiments reveal that the composite COF/CN shows evidently superior photocatalytic performance than individual COF and g-C3N4. The optimized COF–CN (1:10) exhibits a H2 production rate of 12.8 mmol g–1·h–1 under visible-light (λ ≥ 420 nm) irradiation, which is about 62 and 284 times higher than those of COF and g-C3N4, respectively. The apparent quantum efficiency (AQE) of COF–CN (1:10) is about 15.09% under 500 nm light irradiation, which is one of the highest among previous COF- or g-C3N4-based materials. This work provides important strategies for designing and constructing high-efficiency heterojunction photocatalysts with multidimensional features.

研究领域: 材料科学 · 光化学 · 催化 · 纳米技术
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS · 2023 · IF 5.2

Peroxydisulfate nonradical activation on CC engineered g-C3N4: Electron transfer mechanism for selective degradation of organic contaminants

Xinfei Zhang,Xiaobo Jia,Jianhui Zhan,Bin Han,Nan Zhang,Honghao Xie,Feilong Li,Yuan Zhang

The activation of peroxydisulfate (PDS) by g-C 3 N 4 -based catalysts has captured considerable interest; however, the oxidation prowess falls short of expectations, and the inherent processes remain enigmatic. Herein, a novel C C engineered g-C 3 N 4 (CCN) was successfully developed via a one-step thermal polymerization method for the activation of PDS. Our findings revealed that the CCN/PDS system selectively degraded various organic contaminants, operated effectively across a wide pH range (3−9), and maintained high performance in the presence of common water impurities. Experiments and theoretical calculations indicated that the electron transfer process (ETP) was the primary mechanism for phenol degradation. The introduction of C C led to charge redistribution and improved conductivity in g-C 3 N 4 . This enhancement strengthened PDS adsorption at electron-deficient carbon sites and bolstered electron transfer between PDS and organic contaminants. Moreover, a nonradical pathway predicated on ETP emerged when phenol, PDS, and CCN were present, propelled by differences in molecular orbital energies. This study not only deepens our understanding of PDS activation through the ETP but also introduces a novel strategy for the removal of organic contaminants from water.

研究领域: 环境科学 · 材料科学 · 化学工程 · 水处理
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Journal of Environmental Chemical Engineering · 2021 ·Vol. 9 ·期 4 ·105292 · IF 5.909

0D/1D Z-scheme g-C3N4 quantum dot/WO3 composite for efficient Cr (VI) photoreduction under visible light

Jie Zhou,Wenyi Cai,Jing Ding,Hui Wan,Guofeng Guan

The appropriate construct of Z-scheme heterostructure composite with high photocatalytic activity has created new opportunities for environmental protection. Herein, graphitic carbon nitride quantum dots/tungsten trioxide (CNQDs/WO 3 ) was firstly fabricated using CNQDs decorated onto the surface of WO 3 nanorod grown along the [110] orientation in hydrothermal environment to construct a Z-scheme heterostructure composite. By various characterization methods, the crystal structure, micro morphology, atomic valence state and surface functional groups of the catalyst were systematically revealed. The results indicated that Z-scheme heterojunctions between CNQDs and WO 3 were successfully constructed. Compared with pure WO 3 , CNQDs/WO 3 exhibited prominent photoreduction performance under visible light irradiation. The optimal 5% CNQDs/WO 3 could reduce almost 100% Cr (VI) under acidic condition with the best photocatalytic activity within 90 min. More than this, 5% CNQDs/WO 3 also displayed excellent stability and recyclability even after five cycles of photoreduction experiments. Based on the free radical quenching experiments, the possible photoreduction reaction mechanism had been proposed in detail. The Z-scheme heterostructure provided the possibility of the generation, rapidly transfer and efficient separation of photogenerated electrons, which were major active species in the Cr (VI) photoreduction process.

研究领域: 环境催化 · 材料化学 · 纳米科技 · 光催化 · 环境污染治理 · 半导体异质结
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