OPTICAL MATERIALS
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2022
·
IF 3.754
Shirong Kang,Hao Zhang,Mingyu Dou,Gaimei Gao,Hongjie Zhu,Hua Yang,Dacheng Li,Jianmin Dou
The heterojunction structure with CdS@g-C 3 N 4 photocatalyst was obtained via a simple microthermal chemical in-situ deposition method. The catalyst CdS@g-C 3 N 4 (weight ratio of 1:3) maintained excellent degradation activity to 10 ppm tetracycline (TC) after four cycles due to Z-scheme electron transport mechanism, which was demonstrated through several methods, and the photo-corrosion of CdS was inhibited successfully own to this electron transfer paths. Microscope images showed CdS nanoparticles were uniformly distributed on g-C 3 N 4 nanosheets , such surface morphology provided numerous active sites and excellent adsorption performance for photodegradation process. Mechanism study demonstrated the high energy active species including h + , •O 2 − and •OH take part in the degradation process. Through the mass spectrometry analysis , intermediate products and degradation pathway were inferred on TC during photodegradation process. In addition, this study proved the extremely low toxicity of TC aqueous solution after degradation, there was special significance for ecological and environmental protection. This work provided a reference for the design of the Z-scheme photocatalyst and synthesis of catalysts at low temperature (80 °C), and it has application potential in the treatment of water pollution.
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ANALYTICAL AND BIOANALYTICAL CHEMISTRY
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2022
·Vol. 414
·期 13
·3755-3763
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IF 4.478
Wu Shujie,Wang Songen,Li Zongbing,Wu Chun,Ma Dik-Lung,Miao Xiangmin
In this work, we synthesized an iridium(III) complex and studied its selective ability to interact with a specific G-quadruplex DNA sequence (GTGGGTAGGGCGGGTTGG). Results showed that the iridium(III) complex exhibits high selectivity for the G-quadruplex DNA and could be used as an efficient electrochemiluminescence (ECL) probe in a switch-on assay format for the detection of double-stranded DNA (dsDNA). To construct the assay, a hairpin-structured capture probe (CP) which was modified by thiol at its 3′ end and contained the G-quadruplex sequence at its 5′ end was firstly immobilized on a gold electrode. Upon the specific recognition of the dsDNA sequence with the corresponding CP, the hairpin structure of the CP was opened to free G-quadruplex sequence, forming the G-quadruplex structure with the assistance of K + . Then, the iridium(III) complex was able to specifically interact with the G-quadruplex to produce an obvious ECL signal that was proportional to the dsDNA concentration. Notably, this iridium(III) complex/G-quadruplex-based strategy was universal and was not limited to the analysis of DNA using specific sequences, thus opening a new avenue for the application of the G-quadruplex-selective iridium(III) complex in the field of ECL.
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CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Yang Li,Qiao Yin,Yingshan Zeng,Zhi Liu
The core of realizing the effective CO 2 conversion by solar energy is to develop a stable photocatalyst with high CO 2 adsorption capacity and high charge separation efficiency. In this work, a hollow spherical Z-scheme SnS 2 /g-C 3 N 4 /C (SCC) photocatalyst is successfully constructed by a morphology-inherited strategy. Biomass mabospores are utilized as both the precursor for formation of hollow spherical structure and carbon source, and the g-C 3 N 4 and SnS 2 nanosheets tightly anchor on the surface of mabospores-derived carbon spheres. The Z-scheme SCC heterostructure exhibits 5.5 times activity enhancement on CO 2 photoreduction to CO with a high evolution rate up to 40.86 μmol∙g −1 ∙h −1 . Examined by various photoelectrochemical analysis, the boosted photocatalytic activity originates mainly from the construction of hollow spherical Z-scheme heterojunction, providing the more preferable basic sites for CO 2 adsorption, promoting the separation efficiency of electron-hole pairs, as well as increasing the reductionability of electrons in conduction band of g-C 3 N 4 . The formed internal electric fields between the g-C 3 N 4 and SnS 2 can also further reinforce the spatial separation of photogenerated charge carriers. Theoretical calculations further verify that the SCC Z-scheme heterostructure can effectively decrease the energy barriers of formed intermediates, especially the crucial COOH*, and thus leading to the facile conversion of CO 2 -to-CO. This work induces a new strategy to construct g-C 3 N 4 -based Z-scheme heterojunction assisted by versatile biomasses with optimized structure and enhanced photoelectrochemical merits for efficient CO 2 conversion into chemical fuels.
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Journal of Environmental Chemical Engineering
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2022
·
IF 7.968
Yaxi Tian,Yan Gao,Qiongqiong Wang,Zhaojin Wang,Rongfeng Guan,Wenyan Shi
Graphitic carbon nitride (g-C 3 N 4 ) photocatalysts are used to achieve photocatalytic activity under visible light, but they suffer from an unprecedented bottleneck period. These photocatalysts have many intrinsic shortcomings, such as their small specific surface area and inefficient separation rate of photogenerated electron-hole pairs. Therefore, changing the morphology and structure of g-C 3 N 4 are essential challenges in addressing these shortcomings. Herein, we propose a novel one-pot method for constructing porous ultrathin g-C 3 N 4 nanosheets . Melamine and potassium gluconate were effectively combined via a supramolecular assembly strategy. As a gas template, potassium gluconate decomposes to produce CO 2 at high temperature. This novel potassium gluconate-cooperative pore generation on g-C 3 N 4 nanosheets method is proposed for the first time. As a result, the PCN-1.4 (the optimum sample of porous ultrathin g-C 3 N 4 nanosheets) photocatalyst has a large surface and a porous layer structure (67.95 m 2 g −1 , 0.3594 cm 3 g −1 ) with abundant nitrogen defects. Furthermore, the porous ultrathin g-C 3 N 4 nanosheets prepared by this method not only have good performance in hydrogen production , but also in TC degradation. On the one hand, the PCN-1.4 sample exhibits an excellent hydrogen production efficiency (2323 μmol.g −1 h −1 ) that is 12 times that of bulk g-C 3 N 4 (192 μmol g −1 h −1 ). On the other hand, compared to the tetracycline hydrochloride degradation efficiency of bulk g-C 3 N 4 of 22 %, PCN-1.4 exhibits a higher degradation rate as high as 83 %. In summary, a new pathway for the generative pore-making is provided to prepare other porous materials.
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JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY
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2022
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IF 5.141
Wenjing Wang,Xin Xin,Ke An,Yao Chen,Zhanfeng Zhao,Jiangdan Tan,Dong Yang,Zhongyi Jiang
Graphite carbon nitride (g-C 3 N 4 ) has a huge application potential in the photocatalysis field due to its unique conjugated structure. Inspired by the mussel adhesion protein, the cPTA/CNT/CNU (cPTA, carbonized poly(tannic acid); CNT, g-C 3 N 4 prepared by thiourea); CNU, g-C 3 N 4 prepared by urea) nanorod was synthesized by using PTA as the adhesive and template, and thiourea and urea as g-C 3 N 4 precursors. The CNT/CNU isotype heterojunction is assembled on the surface of porous cPTA nanorod, which effectively solves the problem of high photogenerated electron-hole recombination of pure g-C 3 N 4 . The optimal cPTA/CNT/CNU photocatalyst can degrade 95% of rhodamine B (RhB) within 1 h under visible light, which is much higher than CNT, CNU and CNT/CNU. With the conduction band potential difference of cPTA, CNT and CNU, a multistep electron transfer path forms in the cPTA/CNT/CNU, which can accelerate the electron transfer through the interface, thereby increasing the photocatalytic activity.
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TALANTA
·
2022
·
IF 6.556
Yi Wu,Keren Lu,Fubin Pei,Yanghao Yan,Shasha Feng,Qingli Hao,Mingzhu Xia,Wu Lei
The wide clinical application of d -penicillamine (D-PA) makes it inevitably accumulates in the environment, seriously threatening human health and the ecological environment. To better supervisory control D-PA, a highly sensitive and reliable photoelectrochemical (PEC) sensor based on gold nanoparticles (Au NPs) loaded on graphitic carbon nitride sheet and hexagonal NH 2 -UiO-66 composite (g-C 3 N 4 /Au/NH 2 -UiO-66) was synthesized. Tactfully using the strong bonding between D-PA and Au NPs and the effective carrier separation of Z-scheme heterojunction, the designed g-C 3 N 4 /Au/NH 2 -UiO-66 PEC sensor without an extra recognition unit exhibited a selective and sensitive photocurrent to D-PA. With the aid of UV diffuse reflectance spectra (UV-DRs), electron paramagnetic resonance (EPR) characterization, and free radical capture experiments, the electron transfer path of the PEC sensing system was deduced. The proposed g-C 3 N 4 /Au/NH 2 -UiO-66 PEC-based sensor achieved a low detection limit of 0.0046 μM (S/N = 3) with a wide linear response ranging from 10 nM to 400 μM. In addition, its good stability and selectivity also laid a good foundation for practical applications.
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CHEMICAL ENGINEERING JOURNAL
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2022
·
IF 16.744
Yang Huang,Xi Luo,Yini Du,Yu Fu,Xujing Guo,Changwu Zou,Yue Wu
The Fenton-like process provides a promising method to produce reactive radicals for the degradation of refractory organic pollutants in environmental remediation. In this study, the iron-doped g-C 3 N 4 (CNF) coupled with H 2 O 2 was applied to enhance the degradation of carbamazepine (CBZ). And the role of CNF was elucidated by experiment and density functional theory (DFT) calculations. The largest CBZ removal efficiency of 99.02% was achieved in acid condition (pH = 3) with the addition of 0.5 g/L 14% CNF and 50 mM H 2 O 2 . Thirteen intermediates were identified based on high performance liquid chromatography coupled with mass spectrometer (LCMS) and DFT calculations. The degradation products of CBZ were mainly protein-like materials with a low humification degree. During the degradation process, H 2 O 2 was preferentially adsorbed on the active Fe-O site of CNF by hydrogen bonding, hence the promoted electron transfer from H 2 O 2 to Fe(III) contributed to the generation of Fe(II). Certain deformation of H 2 O 2 was observed that the O-O bond length increased to about 1.51 Å. As a result, large amounts of radical species (·OH) were generated by H 2 O 2 decomposition, which was responsible for attacking the CBZ molecules and proceeding the degradation reaction.
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JOURNAL OF POROUS MATERIALS
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2022
·Vol. 29
·期 5
·1431-1440
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IF 2.523
Zhang Shixian,Rong Xinshan,Sun Ting,Gao Ping,Liu Jun,Qiu Xuchun,Zhou Xiangtong,Wu Zhiren
An energy-efficient and environmentally friendly nitrogen fixation process is urgently needed to solve problems of high energy consumption and high emissions in the traditional ammonia industry. In this work, a Z-scheme porous g-C 3 N 4 /ZnFe 2 O 4 photocatalyst was synthesized, characterized and employed for N 2 photofixation. Temperature programmed desorption characterization confirmed that the adsorption capacity of nitrogen was improved for the porous structure. From N 2 photofixation evaluation experiments, the highest ammonia production efficiency can reach 147.33 μmol/L within 120 min. Photocatalytic performance is greatly improved because of the increasing of specific surface areas, enhancement of N 2 adsorption ability and synergistic effect of Z-scheme photocatalytic system. In the ammonia production process of the research, visible light is used as energy; N 2 and H 2 O are used as raw materials, which possesses a good application potential due to the advantages of being energy-efficient, environmentally friendly and pollution-free.
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POLYMER BULLETIN
·
2022
·Vol. 80
·期 4
·4443-4458
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IF 2.843
Zheng Yunxiang,Wang Xiangpeng,Zhang Chunxiao,Zong Lina
Here, copolymerization of acrylic acid (AA) and acrylamide (AM) onto chitosan (CTS) was performed using 2,2'-azobis[2-(2-imidazolin-2-yl)propane] dihydrochloride (VA-044) as the initiator and tetraallylammonium bromine (TAAB) as the crosslinker. The structure of the superabsorbent was characterized via Fourier transform infrared spectroscopy, thermogravimetric analysis, scanning electron microscopy, and atomic force microscopy. The reaction conditions were optimized by an orthogonal experiment, and the water absorbency in different solutions was investigated at 80 ℃. The optimal conditions for the preparation of P(AA-AM)/CTS were as follows: The mass ratios of AM to AA, CTS to AA, VA-044 to AA, TAAB to AA were 20, 7, 0.05, 0.18%, respectively. The superabsorbent showed excellent temperature resistance, and the swelling ratio reached 371.2 g/g in distilled water at 80 ℃. Next, the sensitivity of P(AA-AM)/CTS to various salt concentrations was measured and the results showed that P(AA-AM)/CTS was most sensitive to BaCl 2 , whereas KI had the least influence on water absorbency. Additionally, P(AA-AM)/CTS had different swelling capacities in various pH solutions. The gel showed excellent pH responsiveness; a pH reversible property was observed between pH 2 and 7 as well as pH 7 and 12.
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CRYSTENGCOMM
·
2022
·Vol. 24
·期 28
·5141-5148
·
IF 3.756
Yan Ma,Dianjun Chi,Yuping Tao,Shengjun Liu,Lei Dong,Yu Chen,Lifang He,Kui Zhang
Catalysts with low cost, high efficiency, and no need for precious metal cocatalysts are the key to realizing the maximum utilization of solar energy-efficient hydrogen (H2) production. In this study, a series of graphitic carbon nitride-derived catalysts (g-C3N4/CoP@C) were successfully obtained by in situ phosphating of g-C3N4/Co-BDC. A CoP@C cocatalyst developed with Co-BDC nanosheets as precursors can accelerate the H2 generation of g-C3N4. The close interface between CoP@C and g-C3N4 increased the electron–hole separation efficiency. Moreover, the CoP@C surface carbon accelerated electron transfer and increased the light absorption range. The prepared g-C3N4/CoP@C composite material exhibited H2 production capability up to 1968 μmol g−1 (3 h), approximately 129.9 times that of g-C3N4. Therefore, the CoP@C cocatalyst is proposed as an alternative to non-precious metal cocatalysts based on the findings of the study.
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CHEMOSPHERE
·
2022
·
IF 8.943
Chong Liang,Mingyu Cui,Wei Zhao,Linyang Dong,Shangshang Ma,Xutang Liu,Dingkai Wang,Zhijie Jiang,Fei Wang
Photocatalytic technology has been considered as a promising method to alleviate environmental pollution owing to the dual characteristics of redox. The novel V-based H 5 PMo 10 V 2 O 40 (HPA-2) photocatalyst with Z-scheme heterostructure was constructed. The energy level of HPA-2 matches well with CdS and g-C 3 N 4 (CN) according to Mott-Schottky and UV–Vis diffused reflectance tests, which allows the efficient separation of photogenerated electrons. The optimized CdS/HPA-2/CN showed superior ability in Rhodamine B (RhB) degradation and reduction of Cr (Ⅵ) under visible light irradiation. The maximum rate constant reached 0.092 min −1 for RhB degradation at 60 min and 0.260 min −1 for Cr (Ⅵ) reduction at 20 min, respectively. The photocatalytic mechanism was analyzed by adding scavengers. The effect of active species for RhB degradation was determined as h + > ·O 2 − > ·OH, while ·O 2 − and e − were essential for the reduction of Cr (Ⅵ). Besides, cyclic tests exhibit excellent repeatability and stable structure of CdS/HPA-2/CN after four cycles. Meanwhile, the detailed degradation process of RhB involving de-ethylation, hydroxylation, substitution and decarboxylation was determined according to LC-MS and evaluated by Fukui function calculation. Furthermore, total organic carbon content decreased to 6.2% of the initial value. In this work, as an electron mediator, HPA-2 provides the inspiration for construction of Z-scheme heterojunction , and CdS/HPA-2/CN exhibits enormous potential in the environmental remediation by photocatalysis .
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TALANTA
·
2022
·
IF 6.556
Junyang Chen,Mengke Wang,Chenyu Zhou,Jiabao Zhang,Xingguang Su
Specific and cost-effective methodologies for human papillomavirus (HPV) gene detection are significant for clinical diagnosis and cancer control. Herein, a label-free and fluorimetric/colorimetric dual-mode sensing strategy was developed for the quantitative determination of HPV DNA based on the integration of fluorescent DNA-silver nanoclusters (DNA/AgNCs) and G-quadruplex/hemin DNAzyme. The fluorimetric sensing strategy was based on the phenomena that the fluorescence enhancement of DNA/AgNCs obtained in proximity of guanine-rich DNA sequences and the photoinduced electron transfer (PET) effect between the electron donor (DNA/AgNCs) and electron receptor (G-quadruplex/hemin). The colorimetric sensing strategy was relied on the peroxidase-like activity of G-quadruplex/hemin DNAzyme. By integrating DNA/AgNCs and DNAzyme, this dual-mode strategy could produce two independent signals to improve the analytical diversity and accuracy. Under optimized conditions, the fluorimetry and colorimetry of the strategy displayed a linear range of 0.01–4 and 0.02–4 nM, with the low detection limit of 2.3 and 5.2 pM, respectively. Additionally, this dual-mode strategy has been successfully applied to HPV DNA analysis in different real samples with excellent results. Moreover, the sensing platform could be developed for different HPVs DNA assay by only adjusting the recognition sequence, which provided a universal strategy for various kinds of virus analysis.
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