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Journal of Physical Chemistry C · 2021 · IF 4.126

Real-Time Adsorption and Photodegradation Investigation of Dye Removal on g-C3N4 Surface by Attenuated Total Reflectance Induced Evanescent Spectroscopy

Sha Qin,Yan Xiong,Jun Li,Haiqin Wan,Shenwen Fang,Ming Duan,Rui Li,Donghua Liao

In this work, the adsorption and photodegradation performance of dye pollutant methylene blue (MB) on the g-C3N4 surface was real-time investigated based on attenuated total reflectance induced evanescent spectroscopy (ATR-ES). By coating g-C3N4 on a silica optical fiber (SOF) surface coupled to LED, the produced ATR-ES was interacted with MB adsorbed on the g-C3N4 interface. Therefore, the measurement processes were in situ monitored and real-time evaluated according to ATR-ES change. For adsorption investigation with a red-LED, the change of “red” ATR-ES indicated the adsorption process was spontaneous. At the first stage, the fast adsorption was mainly due to electronic attraction. At the second stage, the slow adsorption was mainly due to the π–π interaction. For photodegradation investigation with a UV-LED, the change of “violet” ATR-ES indicated MB was oxidized by a hydroxyl radical (•OH) and superoxide radical (•O2–) to upset adsorption–desorption equilibrium. The surface apparent adsorption rate was 16 times as high as the apparent photodegradation rate constant, which indicated that the photodegradation process was the main rate control step of photocatalytic degradation reaction. The performances were characterized and verified by SEM measurements, zeta potential analysis, XRD analysis, FTIR investigation, and fluorescence imaging. By utilizing ATR-ES properties on the SOF surface, the adsorption-degradation interaction was continuously real-time monitored.

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Nano Research · 2021 ·Vol. 14 ·期 7 ·2363-2371 · IF 8.897

Fabrication of magnetically recyclable yolk-shell Fe3O4@TiO2 nanosheet/Ag/g-C3N4 microspheres for enhanced photocatalytic degradation of organic pollutants

Lv Yan,Yue Lin,Khan Imran Mahmood,Zhou You,Cao Wenbo,Niazi Sobia,Wang Zhouping

Herein, we report the fabrication of Fe 3 O 4 @TiO 2 nanosheet/Ag/g-C 3 N 4 (Fe 3 O 4 @ns-TiO 2 /Ag/g-C 3 N 4 ) composite photocatalysts with well-designed hierarchical yolk-shell structure. To endow the composites with fascinating features, multiple functional components are perfectly integrated into the definite structure. The photodegradation experiments of organic pollutants revealed a significant enhancement in photocatalytic activity of developed composites as compared to P25, which is mainly due to the synergetic interaction of the tailored three-dimensional (3D) yolk-shell porous nanostructure, extended sunlight response range, and retarded the recombination probability of photogenerated electrons-holes. More importantly, the hybrid samples exhibited superior magnetic properties due to the magnetic component. The excellent magnetic recyclability and reusability of the photocatalysts are verified by the magnetic hysteresis loop and cyclic photocatalytic degradation experiments, which is significant for the green and sustainable applications of photocatalysts. Considering its remarkable photocatalytic performance and expectant magnetic recyclability, the composite photocatalysts are expected to be a promising candidate to dispose of future environmental issues.

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INTERNATIONAL JOURNAL OF PHARMACEUTICS · 2021 · IF 5.875

Topical application of HA-g-TEMPO accelerates the acute wound healing via reducing reactive oxygen species (ROS) and promoting angiogenesis

Junjun Li,Rong Du,Qiong Bian,Danping Zhang,Siqian Gao,Anran Yuan,Xiaoying Ying,Youqing Shen,Jianqing Gao

During the occurring of cutaneous trauma, increasing oxidative stress response in wound site retards the progress of proliferation phase, impeding sequent efficient wound repair. At the same time, high-quality healing also requires adequate new blood vessels in order to furnish the wound site with a nutrient and oxygen-sufficient environment. Here we synthesized a novel hyaluronic acid (HA) material modified with a peroxidation inhibitor 2,2,6,6-tetramethylpiperidinyloxy (ATEMPO) for prevention of excessive reactive oxygen species (ROS) and promotion of angiogenesis after full-thickness skin excision in rats. Amines in ATEMPO attaching with carbonyls in HA chains was fabricated through N-acylation. The HA-g-TEMPO exerted a ROS-scavenging and angiogenesis-promoting function in vitro . In acute wound rat model, the wound closure efficacy was significantly improved to almost 55% at day 6 in comparison to 49% of HA, and wound sites in initial wound phase was also narrowed down sharply. Moreover, initially formed blood vessels were found in wound sites, further proved the angiogenesis-promoting function of HA-g-TEMPO. More interestingly, wound sites demonstrated an exciting regenerative healing effect which was characterized by marked skin appendages as well as reduced scarring. Therefore, this strategy showed a promising future that could be considered as a reliable and effective method to cutaneous wound healing.

✓ 已验证 DOI PubMed 高影响因子
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES · 2021 · IF 6.953

Combing multiple site-directed mutagenesis of penicillin G acylase from Achromobacter xylosoxidans PX02 with improved catalytic properties for cefamandole synthesis

Anni Li,Cheng Cheng,Weimin Qi,Xin Pan,Xuanping Xu,Xinyu Wang,Chunying Wu,Jianlin Chu,Bingfang He

Penicillin G acylase (PGA) was an important biocatalyst for enzymatic production of second-generation cephalosporin. PGA from Achromobacter xylosoxidans PX02 ( Ax PGA) showed relatively lower identity to Ec PGA (54.9% in α subunit and 51.7% in β subunit), which could synthesize cefamandole in the kinetically controlled N -acylation ( kcNa ). Semi-rational design of Ax PGA and “small and smart” mutant libraries were developed with minimal screening to improve cefamandole production. A triple mutant αR141A/αF142I/βF24G by combining the mutational sites (βF24, αR141, and αF142) from different subunits of Ax PGA showed better performance in cefamandole production, with 4.2-fold of improvement in the (k cat /K m ) AD value for activated acyl donor ( R )-Methyl mandelate. Meanwhile, the (k cat /K m ) Ps value for cefamandole by mutant αR141A/αF142I/βF24G was sharply dropped by 25.5 times, indicating its highly synthetic activity and extremely low hydrolysis of cefamandole. Strikingly, the triple mutant αR141A/αF142I/βF24G could form cefamandole with a yield of 85% at an economical substrate ratio (acyl donor/nucleophile) of 1.3:1 (82% at 1.1:1), which advanced the greener and more sustainable process of cefamandole production than the wild type. Furtherly, the improved synthetic ability and lower hydrolysis of cefamandole by mutant were rationalized using molecular docking.

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ACS Applied Materials & Interfaces · 2021 · IF 9.229

Stitching Graphene Sheets with Graphitic Carbon Nitride: Constructing a Highly Thermally Conductive rGO/g-C3N4 Film with Excellent Heating Capability

Yanyan Wang,Xian Zhang,Xin Ding,Ya Li,Bin Wu,Ping Zhang,Xiaoliang Zeng,Qian Zhang,Yuhang Du,Yi Gong,Kang Zheng,Xingyou Tian

Driven by the evolution of electronic packaging technology for high-dense integration of high-power, high-frequency, and multi-function devices in modern electronics, thermal management materials have become a crucial component for guaranteeing the stable and reliable operation of devices. Because of its admirable in-plane thermal conductivity, graphene is considered as a desired thermal conductor. However, the promise of graphene films has been greatly weakened as the existence of grain boundaries lead to a high extent of phonon scattering. Here, a stitching strategy is adopted to fabricate an rGO/g-C3N4 film, where 2D g-C3N4 works as a linker to covalently connect adjacent rGO sheets for expanding the size of graphene and forming an in-plane rGO/g-C3N4 heterostructure. The in-plane thermal conductivity of the rGO/g-C3N4 film reaches 41.2 W m–1 K–1 at a g-C3N4 content of only 1 wt %, which increased by 17.3% compared to pristine rGO. The interfaced thermal resistance between rGO and g-C3N4 is further examined by non-equilibrium molecular dynamics simulations. Furthermore, owing to the unique light absorption and welding ability of g-C3N4, the rGO/g-C3N4 film presents superior solar-thermal and electric-thermal responses to controllably regulate the chip temperature against overcooling. This work provides a facile approach to construct a large-sized rGO sheet and combines heat dissipation and heating capability in the same thermal management material for future electronics.

CAS / MDL: 108-78-1
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FOOD CHEMISTRY · 2021 · IF 7.514

Rapid, ultrasensitive and non-enzyme electrochemiluminescence detection of hydrogen peroxide in food based on the ssDNA/g-C3N4 nanosheets hybrid

Zhijun Liu,Li Wang,Pengfei Liu,Kairen Zhao,Shuying Ye,Guoxi Liang

Hydrogen peroxide (H 2 O 2 ) is usually used as a fungicide in food, it is carcinogenic, accelerates aging or inducing toxic effects such as cardiovascular disease. Herein, to meet the demand for effective and fast detection of H 2 O 2 in food, a novel non-enzymatic electrochemiluminescence (ECL) sensor based on single-stranded DNA (ssDNA)/g-C 3 N 4 nanosheets (NS) was established. The ssDNA/g-C 3 N 4 NS hybrid was prepared by simple mixing g-C 3 N 4 NS and ssDNA solution together. The prepared ssDNA/g-C 3 N 4 NS exhibited improved peroxidase-like activity and was modified on a glassy carbon electrode to catalyze the ECL reaction of luminol-H 2 O 2 to amplify the luminescence signal. Under the optimized conditions, the proposed sensor exhibits high sensitivity with a limit of detection (LOD) as low as 33 aM H 2 O 2 , which is much lower than the vast majority of reported methods. This method enables the reliable responding to H 2 O 2 from the milk samples within 1 min.

CAS / MDL: 108-78-1
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SENSORS AND ACTUATORS B-CHEMICAL · 2021 · IF 7.46

Double-stranded DNA nanobridge enhanced fluorescence of crystal violet/G-quadruplex complex for detection of lead ions and crystal violet

Jiao Zhou,Min Qing,Yu Ling,Lei Wang,Nian Bing Li,Hong Qun Luo

DNAzyme and G-quadruplex are purposed as universal recognition elements to achieve multi-functional signal amplification and readout, showing great potential in the design of biosensors and nanodevices. Herein, the single-stranded DNA (ssDNA) opens the dumbbell-shaped hairpin probes, the generated double-stranded DNA (dsDNA) is constructed as a nanobridge, and the released G-rich sequence is folded into a G-quadruplex village. The fluorescence of crystal violet/G-quadruplex complex villages is enhanced by the dsDNA nanobridge connections. Under the excitation wavelength of 580 nm, the fluorescence emission intensity at 624 nm exhibits a good linearity with the concentration of crystal violet (CV) in the range of 10–250 nM, which can be used for sensitive detection of CV . Additionally, combined with Pb 2+ -dependent DNAzyme, a platform for quantitative detection of Pb 2+ is established. In the concentration range of 5 nM – 25 μM, the fluorescence signal increases with the increase of Pb 2+ concentration. The quantitative detection limit of Pb 2+ by this method is 5 nM, and it possesses good selectivity and recovery for Pb 2+ in a variety of water samples. More importantly, the platform can sensitively detect various metal ions by changing the DNAzyme sequence. It has potential application in the field of environmental monitoring.

CAS / MDL: 77-86-1
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CHEMICAL ENGINEERING JOURNAL · 2021 · IF 13.273

Three-Dimensional g-C3N4/NH2-UiO-66 graphitic aerogel hybrids with recyclable property for enhanced photocatalytic elimination of nitric oxide

Zhou Zhou,Dongyun Chen,Najun Li,Qingfeng Xu,Hua Li,Jinghui He,Jianmei Lu

In order to fix the photocatalyst and enhance the efficiency of NO degradation, a three-dimensional (3D) g-C 3 N 4 /NH 2 -UiO-66-rGO (CN/NU6-rGO) aerogel was devised and fabricated via solvothermal reaction and boiling-water bath. Herein, a type-II heterojunction was formed at CN/NU6 composite, and then, the composite was coupled with rGO. The resulting material significantly enhanced the nitric oxide (NO, 600 ppb) removal efficiency under visible-light irradiation. Optimizing the content of CN and rGO to a suitable mass ratio can increase the removal efficiency by 65.4%, which is 2.34 times that of pure NU6. This result is attributed to the construction of type-II heterojunction and the charge transport properties of rGO. The involvement of rGO not only provided extra pathways for charge transfer to prevent electron–hole pairs from recombining, but also fixed the catalyst. Moreover, the hybrid aerogel excellently reduced the harmful by-product NO 2 . Cycling experiments, along with transient photocurrent response measurements, verified that CN/NU6-rGO had excellent potential for recyclable and sustainable. This work might shed light on the construction of suitable photocatalytic systems with significant improvement of NO removal and convenient storage of catalyst.

CAS / MDL: 10026-11-6
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ANALYTICAL AND BIOANALYTICAL CHEMISTRY · 2021 ·Vol. 413 ·期 8 ·2071-2079 · IF 4.157

A low-background fluorescent aptasensor for acetamiprid detection based on DNA three-way junction-formed G-quadruplexes and graphene oxide

Zhao Yunwei,Zhang Hui,Wang Ying,Zhao Yanfang,Li Yaowei,Han Lei,Lu Lihua

A simple fluorescence detection platform has been established for acetamiprid assay based on DNA three-way junctions (TWJs), which can triple the fluorescence signal without any other amplification. It is designed with three single-stranded DNAs (ssDNA), each of which contains one-third or two-thirds of the G-quadruplex sequence at each end. Upon the addition of acetamiprid, the conformation of the aptamer-containing double-stranded DNA (dsDNA) changes from its original conformation and releases a strand of ssDNA. This ssDNA, with the other two ssDNAs, can assemble into DNA TWJs, and the three pairs of the branched ends of the DNA TWJs are adjacent to each other, allowing them to form three units of G-quadruplexes. Hence, the fluorescence of N -methyl mesoporphyrin IX (NMM) is lighted by the nascent G-quadruplexes. Graphene oxide (GO) is then added to minimize the detection background by absorbing the free NMM and non-target-induced ssDNA. The proposed strategy can assay acetamiprid in a wide linear range of 0–500 nM with a detection limit of 5.73 nM. More importantly, this assay platform demonstrates high potential for acetamiprid assay in food control and environmental monitoring.

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JOURNAL OF MOLECULAR LIQUIDS · 2021 · IF 6.165

Highly efficient removal of organic pollutants from wastewater using a recyclable graphene oxide membrane intercalated with g-C3N4@TiO2-nanowires

Yi Huang,Gen Zhu,Kun Zou,Fei Tian,Thakur Prasad Yadav,Hui Xu,Guohai Yang,Haitao Li,Lulu Qu

Membrane fouling has been a major challenge in the practical application of membrane technology for wastewater treatment and purification. In this study, a reusable membrane composed of g-C 3 N 4 @TiO 2 -nanowires modified graphene oxide (GO/CN@TNWs) was successfully fabricated through electrostatic interactions and a vacuum filtration-assisted self-assembly process. The as-fabricated membrane possessed higher photocatalytic activity than the pure TNWs under simulated solar light exposure, attributing to the introduction of GO with high absorption and carrier mobility, and the synergistic effects of TNWs and CN. Furthermore, the π-π stacking interactions between GO and organic pollutant molecules contribute to the excellent enrichment efficiency of GO/CN@TNWs membrane (98.77%) toward tetracycline hydrochloride (TCH). Room-temperature ESR studies indicate that the GO/CN@TNWs membrane can generate more superoxide radical, hydroxyl radical and hole species for photocatalytic degradation. Therefore, the GO/CN@TNWs membrane may be used for TCH removal from waste water and the excellent solar-light-driven photocatalytic performance endows GO/CN@TNWs membrane absorbents with recycling abilities for the realization of large-scale wastewater purification.

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ACS Applied Energy Materials · 2021 · IF 6.024

Embedding 1D WO3 Nanotubes into 2D Ultrathin Porous g-C3N4 to Improve the Stability and Efficiency of Photocatalytic Hydrogen Production

Fang Feng,Hongfeng Hua,Lutao Li,Rongxi Xu,Jiayu Tang,Dejiang Dong,Jian Zhang,Xing’ao Li

Recently, two-dimensional (2D) g-C3N4 has attracted great interest for visible-light-driven H2 production. Thinning, doping, and reticulation have been demonstrated as effective strategies to improve the efficiency of photocatalysis, but are a challenge for structural stability. Herein, a targeted method was implemented by embedding the one-dimensional (1D) WO3 nanotubes matrix into the frameworks of 2D porous g-C3N4 to form a porous P-doped g-C3N4 nanosheets/WO3 nanotubes (PCNS/WNT) by a flexible electrostatic self-assembly process. As a visible-light-sensitive photocatalyst, the as-prepared hybrids exhibited impressive performance for hydrogen generation, which was attributed to the advantages of synergetic mechanism owing to a higher specific surface area, more reaction active sites, enhanced light absorption, and a better photogenerated carrier separation. Interestingly, the insertion of 1D WO3 nanotubes not only accelerates electrons transfer along the 1D channel but also provides robust support for 2D porous g-C3N4 architecture. As a result, the maximum photocatalytic H2 evolution rate of PCNW-50 is 547 μmol g–1 h–1, which is about four times higher than that of pure PCNS, and there is no significant reduction of H2 production after five cycles. Moreover, this 2D/1D PCNS/WNT hybrid was first reported in the area of photocatalytic hydrogen evolution and provides ideas for designing novel stable architecture of photocatalyst.

CAS / MDL: 2041-14-7
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SEPARATION AND PURIFICATION TECHNOLOGY · 2020 · IF 5.774

Efficiently enhanced visible-light photocatalytic activity by in situ deposition of Ag@AgBr on g-C3N4/Fe3O4 magnetic heterogeneous materials

Xiao Zhang,Bin Ren,Xi Li,Yanhua Xu,Biming Liu,Peng Yu,Yongjun Sun,Danhua Mei

In this study, graphitic carbon nitride (g-C 3 N 4 ) (CN) was conveniently and environmentally modified into a stable and easily recyclable photocatalyst for the high removal efficiency of dye contaminants in water. Magnetic carrier (CN/Fe 3 O 4 ) and heterojunction photocatalysts (Ag@AgBr/CN/Fe 3 O 4 ) were prepared by ultrasonic and in situ deposition of Fe 3 O 4 and Ag@AgBr nanoparticles on the CN , respectively, and characterized by the surface structure, optical, and electrochemical properties. The effects of different catalysts, silver loading, catalyst dosage, and different aeration conditions on the photocatalytic degradation of RhB were investigated. Results exhibited that the removal rate of RhB by Ag@AgBr/CN/Fe 3 O 4 reached 96% within 150 min when the Ag loading was 5%, the catalyst dosage was 0.4 g/L, and the aeration was air. Furthermore, the degradation rate constant was 17.3 × 10 −3 min −1 , which was 4.3 and 3.4 times higher than that of CN and CN/Fe 3 O 4 , respectively. The stability study demonstrated that Ag@AgBr/CN/Fe 3 O 4 had almost no risk of Ag and Fe leakage and showed high stability. Mechanism study indicated that the construction of Z-scheme heterojunction between Ag@AgBr and CN and trapping electron by Fe 3+ promoted charge transfer and electron–hole pair separation, thus enhancing photocatalytic activity.

CAS / MDL: 106-51-4 108-78-1
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