Solar RRL
·
2021
·Vol. 5
·期 12
·2100559
·
IF 8.582
Hong-Hong Zhang,Zi-Chun Zhou,Yu-Jie Dong,Li Zhang,Hong-Yan Chen,Dai-Bin Kuang
Utilizing halide perovskites for photocatalytic aromatic C( sp 3 ) H bond activation remains a great challenge due to the serious recombination of photogenerated charge carriers and slow reaction dynamics of the materials themselves. Herein, a lead-free perovskite-based hybrid of Cs 3 Sb 2 Br 9 /g-C 3 N 4 nanosheet is constructed and applied for photocatalytic aromatic C( sp 3 ) H bond activation, which shows enhanced photocatalytic performance. By introducing ultrathin g-C 3 N 4 nanosheets as the heterogeneous nucleation sites, size-reduced and well-dispersed Cs 3 Sb 2 Br 9 nanocrystals can be obtained. The as-formed close contact and high-quality heterointerface between Cs 3 Sb 2 Br 9 and g-C 3 N 4 provides pathways for fast charge transfer which is beneficial to improve the separation efficiency of photogenerated electron−hole pairs. Under visible light irradiation, the Cs 3 Sb 2 Br 9 /g-C 3 N 4 hybrid photocatalyst can effectively oxidize toluene toward benzaldehyde and benzyl alcohol with a total conversion rate of 8346.8 μmol g −1 h −1 , which is 26.6- and 6.0-fold that of pure g-C 3 N 4 and Cs 3 Sb 2 Br 9 , respectively. This work demonstrates the potential of all-inorganic lead-free halide perovskite-based heterostructures for photocatalytic organic reactions.
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高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
·
2021
·
IF 7.46
Pengcheng Zhao,Linzi Huang,Hui Wang,Chenxi Wang,Jia Chen,Pingping Yang,Meijun Ni,Chao Chen,Chunyan Li,Yixi Xie,Junjie Fei
Baicalin (Bn) obtained from natural plants has been found to exhibit significant antiviral activity against Severe Acute Respiratory Syndrome Coronavirus 2 (SARS-CoV-2). Herein, a novel ultrasensitive Bn electrochemical sensor was proposed based on graphitized carbon-nitride - single-walled carbon nanotube nanocomposites (C 3 N 4 -SWCNTs), reduced graphene oxide (rGO) and electrodeposited cyclodextrin-metal organic framework (CD-MOF). The sensing nanomaterials were characterized by X-ray diffraction spectroscopy, X-ray photoelectron spectroscopy, Raman spectroscopy, scanning electron microscopy, and transmission electron microscopy. Under optimal conditions, the sensor exhibited sensitive detection of Bn in a wide linear range of 1 × 10 -9 –5 × 10 -7 M with an LOD of 4.6 × 10 -10 M and a sensitivity of 220 A/M, and it showed satisfactory stability and accuracy for detecting Bn in real samples (human serum and bear bile scutellaria eye drops). In addition, the electrochemical reaction sites and redox mechanism of Bn were revealed through electrochemical behavior and density functional theory. This work provided an insightful solution for detecting Bn, and extensive potential applications could be further expected.
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Analytical Methods
·
2021
·Vol. 13
·期 48
·5830-5837
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IF 2.896
Shouhui Chen,Jingguo Yu,Zhen Chen,Zhenzhong Huang,Yonghai Song
The presence of Cd2+, Pb2+, Cu2+ and Hg2+ in drinking-water can be harmful to human health, even if their concentration is fairly low. Hence, it is significant to detect these heavy metal ions in sewage to evaluate the quality of water. Herein, amino-functionalized metal–organic frameworks (NH2-MIL-88(Fe)) embedded with graphitic carbon nitride (g-C3N4) nanosheets and acid-functionalized carbon nanotubes were prepared via a one-pot synthesis. The composite can be directly modified on the surface of glass carbon electrodes without the assistance of Nafion or other binders. The modified glass carbon electrodes can be used to simultaneously detect Cd2+, Pb2+, Cu2+ and Hg2+ in water via square wave stripping voltammetry. The doping of g-C3N4 in the composite, rich in N-containing functional groups, participates in the adsorption of metal ions on the surface of the electrodes. The porous composite provides accommodation room for metals generated by electro-reduction. The detection limit for Cd2+, Pb2+, Cu2+ and Hg2+ is 39.6 nM, 7.6 nM, 11.9 nM, and 9.6 nM, respectively. And the sensitivity for Cd2+, Pb2+, Cu2+ and Hg2+ is 0.0789 mA μM−1 cm−2, 0.4122 mA μM−1 cm−2, 0.2616 mA μM−1 cm−2, and 0.3251 mA μM−1 cm−2, respectively. This work not only enriches the functional design of Fe-MOF materials, but also develops a method for the determination of metal ions using the adsorption sites in g-C3N4.
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APPLIED SURFACE SCIENCE
·
2021
·
IF 6.707
Jianmei Pan,Yahai Zhang,Yi Guan,Yingnan Yan,Hua Tang,Xianglong Liu,Mengdi Wang,Xiangxin Wei
The development of hydrogen (H 2 ) production photocatalyst with low cost, non-precious metal and high-activity for commercial application is a long-term target and challenge. In this work, novel silicon carbide (SiC) nanofibers/graphitic carbon nitride (g-C 3 N 4 ) nanosheets (SiC/CNNS) decorated via multipurpose nickel (Ni) nanoparticles were prepared by an easy heat treatment followed by hydrothermal method. The tight Ni interface layers as cocatalyst and electron transfer mediator can significantly enhance the H 2 production property over SiC/CNNS nanoheterojunctions under light-emitting diode (LED) illumination. The optimal Ni/SiC/CNNS with a mass fraction of 10% Ni loading shows the most superior H 2 -generation rate of 6183 μmol g −1 h −1 , which is approximately 53, 3 and 227 times compared to CNNS, 10 %Ni/CNNS and SiC/CNNS, respectively. The metallic Ni nanoparticles play the leading and multifunctional roles in improving photocatalytic activity, including collecting the photo-generated electrons efficiently, transferring and separating the charge carriers rapidly, facilitating the H 2 -production kinetics and decreasing the overpotentials of surface reactions for H 2 -production. It is highly expected that the multipurpose and non-precious metal cocatalyst to form tight interface layers can supply a simple and universal strategy to design high-efficiency cocatalyst-semiconductor–semiconductor photocatalysts for H 2 production.
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Catalysis Science & Technology
·
2021
·Vol. 11
·期 24
·7963-7972
·
IF 6.119
Anyu Liu,Jianqiang Hu,Jiale He,Xinyue Huang,Na Hu,Yuqin Li,Qingling Huang,Shien Guo,Xin Liu,Zhen Yang,Yong Zhou,Zhigang Zou
O-doped g-C3N4/In2S3 hierarchical heterostructures with a direct Z-scheme mechanism were devised and constructed simply via loading In2S3 nanoflakes on the surface of O-doped g-C3N4 (OCN) hierarchical structures, in situ, employing pre-obtained OCN (prepared by condensation of oxalic acid and urea) and indium(III) dimethyldithiocarbamate (In(dedc)3) as precursors. Analyses of the energy band structure, density functional theory (DFT) computations and DMPO-ESR spin-trapping experiments demonstrate that the formation of a perfect heterointerface with a staggered alignment of band edges between OCN and In2S3 (IS), owing to their close contact, enables photoexcited carriers to migrate via a Z-scheme route, which can maintain the higher reduction and oxidation capability of electrons and holes, respectively. Furthermore, the Z-scheme OCN/IS heterostructures efficaciously facilitate the separation of photogenerated electrons and holes, as demonstrated using PL spectra, transient photocurrent densities and electrochemical impedance spectra (EIS). These lead to the enhanced photocatalytic activity towards reducing Cr(VI) into Cr(III). Besides, the integration of OCN with IS can enhance the responsiveness to visible light based on the results of UV-vis DRS, thereby inducing the formation of more electrons and holes,and also contributing to the improvement of the photocatalytic activity for Cr(VI) reduction. In consequence, all the pre-prepared OCN/IS hybrids possess markedly improved photocatalytic activities for Cr(VI) reduction, relative to pure OCN and pristine IS under visible light (λ > 420 nm) illumination. With the increase in the In(dedc)3 to OCN mass ratio (R), the photocatalytic activities of these OCN/IS hybrids increase first and then decrease. The sample with an optimum R of 0.9 (OCN/IS-0.9) can remove nearly 100% of Cr(VI) after 40 min of illumination, being superior to most of g-C3N4-based and IS-based photocatalysts. Its reaction rate constant for Cr(VI) photoreduction (0.08947 min−1) is 56.7 fold and 8.8 fold higher than that of pure OCN (0.00155 min−1) and pristine IS (0.00913 min−1), respectively. This work affords a deep understanding on designing preeminent Z-scheme photocatalysts towards the degradation of Cr(VI) under visible-light irradiation.
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Nanomaterials
·
2021
·Vol. 11
·期 12
·3341
·
IF 5.076
Yuan Guo,Wanqing Liu,Wei Duan,Siyu Wang,Liqun Jia,Guoqing Zhang,Baolin Zhu,Weiping Huang,Shoumin Zhang
Photocatalytic water splitting for hydrogen generation is a significant pathway for sustainable energy conversion and production. The photocatalysts with a Z-scheme water splitting charge transfer pathway is superior due to the good separation and migration ability of photoexcited charge carriers. Herein, Co3O4/g-C3N4photocatalysts with Z-scheme charge transfer pathway were successfully constructed by an electrostatic interaction-annealing method. The as-prepared Co3O4/g-C3N4ultra-thin nanosheets were tested and analyzed by XRD, EA, ICP, SEM, TEM, AFM, XPS, UV-Vis DRS, PL and photoelectrochemical measurements. Moreover, the influences of fabrication parameters on performance of Co3O4/g-C3N4catalysts were investigated, and 0.5% Co3O4/g-C3N4exhibited the optimal activity. Based on the characterization and catalytic performance, the Z-scheme charge transfer pathway of Co3O4/g-C3N4was established and put forward. To further improve the catalytic performance of Co3O4/g-C3N4, 0.5% Pt was added as a co-catalyst. The obtained Pt/0.5% Co3O4/g-C3N4was recyclable and remained the original catalytic water splitting performance within 20 h. The modification of Co3O4and Pt improved the separation and migration of e−and h+, and induced the increased hydrogen evolution rate of g-C3N4.Keywords:Co3O4/g-C3N4ultra-thin nanosheets;Z-scheme charge transfer pathway;photocatalytic;water splitting;H2evolution
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高影响因子
NEW JOURNAL OF CHEMISTRY
·
2021
·Vol. 45
·期 47
·22123-22132
·
IF 3.591
Jing Liu,Dianming Li,Xiaofeng Liu,Jie Zhou,Hong Zhao,Nü Wang,Zhimin Cui,Jie Bai,Yong Zhao
Hydrogen evolution and dye degradation catalyzed by environmentally benign and inexpensive photocatalyst in aqueous solution is regarded as a promising avenue to effectively address the global energy and environmental crisis. It is difficult for traditional photocatalysts to perform efficient light harvesting, with conducive recycling and promoted charge separation and transport, which limit practical applications in photocatalytic conversion. In this study, a facile template-assisted coaxial electrospinning approach was explored to successfully build close contacted heterojunctions within the interface of g-C3N4 nanosheets and hollow porous TiO2 nanofibers, which significantly increased the separation efficiency of photo-induced electron–hole pairs in the visible-light region. A hollow and porous structure with abundant surface-active sites assisted in inducing multiple light reflection for more efficient light harvesting. Moreover, one dimensional TiO2/g-C3N4 composite nanofibers with a large length-to-diameter ratio would be more attractive for recovery. At the optimal g-C3N4 loading, hollow porous TiO2/g-C3N4-50% nanofibers exhibited the highest rate of hydrogen evolution and RhB degradation. The enhanced photocatalytic performance of hollow porous TiO2/g-C3N4 composite photocatalysts was mainly attributed to the synergistic effect of the hollow porous architecture and heterojunction. This work might make a significant contribution to insight into preparing hollow structure heterogenous nanofiber photocatalysts with improved activities in hydrogen generation and pollutant degradation.
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY
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2021
·
IF 4.464
Jun-Tao Cao,Jing-Lu Lv,Yu-Xiang Dong,Xiao-Jing Liao,Shu-Wei Ren,Yan-Ming Liu
A general spatial-resolved photoelectrochemical (PEC) sensing platform for sensitive and high-throughput protein analysis was developed by integrating CdS@g-C 3 N 4 heterojunction modified rotatable electrodes array with signal antibodies labeled Cu 2 O (Cu 2 O-Ab 2 ) conjugates. The disk substrate containing eight spatial-resolved working electrodes array was fabricated using acid etching treatment method. After stepwise immobilizing CdS@g-C 3 N 4 , capture antibodies (Ab 1 ), varied concentrations of target protein (prostate-specific antigen) and Cu 2 O-Ab 2 conjugates on the corresponding sensing sites, the immunosensor array was prepared completely. Combining the high photoelectric conversion efficiency of the photoactive material with the effective signal probe, the immunosensor exhibits high sensitivity. The proposed spatial-resolved immunosensing platform shows a working range of 1.0 × 10 -11 – 5.0 × 10 -8 g mL −1 with a detection limit of 5.0 pg mL −1 . The method provides a universal paradigm for near-simultaneously detection of multi-batch samples with good specificity and high sensitivity.
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APPLIED SURFACE SCIENCE
·
2021
·
IF 6.707
Qinxue Xiong,Yi Chen,Tiefeng Xu,Zhexin Zhu,Wenxing Chen,Wangyang Lu
In this work, a flexible photocatalytic material (TiO 2 @g-C 3 N 4 -cotton) was obtained using modified graphitic carbon nitride (g-C 3 N 4 -CONH-KH550) for the a connection between the natural cotton supports and titanium dioxide (TiO 2 ) successively. Under the visible light, a valid photocatalytic activity was observed in the degradation of sulfaquinoxaline (SQX) and thiamethoxam. According to the support stability tests and the UV accelerated aging tests, g-C 3 N 4 -CONH-KH550 could shelter the supports with TiO 2 from the oxidation attack by hydroxyl radicals (•OH) generated. The investigation of antibacterial activity showed efficient inactivation of both Escherichia coli ( E. coli ) and Staphylococcus aureus ( S. aureus ). Therefore, TiO 2 @g-C 3 N 4 -cotton showed stronger mechanical performance and much longer lifetime compared with TiO 2 @cotton. The degradation products and processes of substrates were investigated. This paper provides a new idea about the construction of an efficient and stable supported photocatalytic material.
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Journal of Materials Research and Technology-JMR&T
·
2021
·
IF 5.039
Yushuai Chen,Bo Yang,Wenyu Xie,Xueying Zhao,Zhuan Wang,Xintai Su,Chao Yang
Insufficient active sites and fast charge carrier recombination are detrimental to photocatalytic activity of graphitic carbon nitride (g-C 3 N 4 ). In this work, a combination of pore creating with thermal exfoliation was employed to prepare porous g-C 3 N 4 nanosheets for photocatalytic water splitting into hydrogen. Hexadecyl trimethyl ammonium chloride (CTAC) as the soft template promoted the formation of porous g-C 3 N 4 during the thermal condensation of melamine. On further post-synthesis calcination, the porous g-C 3 N 4 aggregates were exfoliated into discrete nanosheets, accompanied by an increase in specific surface area and defects. Optimal porous g-C 3 N 4 nanosheets achieved 3.6 times the photocatalytic hydrogen evolution rate for bulk counterpart. The enhanced photocatalytic activity may be ascribed to TCN-1%CTAC has larger specific surface area, stronger optical absorption intensity and higher photogenerated electron–hole separation efficiency. The external quantum efficiency of TCN-1%CTAC was measured to be 3.4% at 420 nm. This work provides a simple combinatorial strategy for the preparation of porous g-C 3 N 4 nanosheets with low cost, environmental friendliness and enhanced photocatalytic activity.
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CHEMOSPHERE
·
2021
·
IF 7.086
Likun Chen,Kewen Xing,Qikai Shentu,Yifei Huang,Weiyang Lv,Yuyuan Yao
Developing single-atom Fenton-like catalysts with the maximum utilization of active sites present an attractive potential in environmental remediation. Herein, the single-atom Fe and N co-doped hollow carbon microsphere loaded g-C 3 N 4 catalyst (HFeNC-g-C 3 N 4 ) was prepared by an innovative cascade anchoring strategy using polystyrene as the hard template, iron phthalocyanine, polydopamine and urea as the Fe, N and C precursor, in which the in-situ generated g-C 3 N 4 could not only effectively anchor Fe atom to create the well-dispersed Fe-N x active sites, but also accelerate the electron transfer in peroxymonosulfate (PMS) activation. Taking advantages of such sequential protecting strategy, the as-synthesized HFeNC-g-C 3 N 4 catalyst with single-atom Fe-N x active sites, verified by XRD , XPS and HAADF-STEM, could work as an efficient Fenton-like catalyst for PMS activation, which achieved almost 100% removal of 4-chlorophenol (4-CP) in 5 min with the turnover frequency calculated to be 34.6 times higher than that of the homogeneous Fe 2+ catalyst. The mechanism of O 2 •- dominated radical combined with nonradical 1 O 2 pathway was confirmed by quenching experiments and ESR analysis, which might be interrelated to the improvement of pH adaptability and interference immunity of HFeNC-g-C 3 N 4 /PMS system. Overall, the present findings provided an innovation strategy for the synthesis of excellent single-atom Fe based catalyst in wastewater purification.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2021
·
IF 8.128
Yiwei Shan,Ying Guo,Yu Wang,Xiran Du,Jun Yu,Hao Luo,Hui Wu,Bruno Boury,He Xiao,Liulian Huang,Lihui Chen
Using oxygen reduction for the photocatalytic production of hydrogen peroxide (H 2 O 2 ) has been considered a green and sustainable route. In the present study, to achieve high efficiency, graphitic carbon nitride (g-C 3 N 4 ) was obtained using thermal polymerization from a bi-component precursor and was then assembled with cellulose nanofibers . It was found that a small quantity of cellulose nanofibers that generates carbon fibers upon pyrolysis greatly improves the photocatalytic activity compared with that of g-C 3 N 4 alone. The well-defined carbon/g-C 3 N 4 heterojunction-type material exhibits as high as 1.10 mmol L -1 h −1 of photo-production of H 2 O 2 under visible light , which is 4.2 times higher than that yielded by pristine g-C 3 N 4 from a single precursor. A comprehensive characterization of the photocatalyst enables us to delineate the effect of the carbon nanofiber with respect to porosity, electron–hole separation, band gap regulation, and especially the electron transfer pathway. Our results demonstrate that nanocellulose-derived carbon, when precisely assembled with other functional material such as a photocatalyst, is a promising promoter of their activity.
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