Journal of Physical Chemistry C
·
2022
·
IF 4.177
Kang Hu,Ping Liu,Ziqing Zhang,Ji Bian,Guowei Wang,Hongjun Wu,Hui Xu,Liqiang Jing
g-C3N4 is a promising photocatalyst for CO2 conversion owing to its outstanding reduction potential. However, its shallow valence band position and sluggish water oxidation reaction restrict the overall CO2 photoreduction process. Herein, g-C3N4 nanosheets are first doped with B through thermal treatment of mixed NaBH4 and subsequently modified with highly dispersed Ru-oxo clusters by using tailored chitosan oligomers. The optimal Ru-oxo modified B-doped g-C3N4 exhibits an exceptional photocatalytic CO2 conversion rate with 22-fold improvement compared with pristine CN. Based on the results of electron paramagnetic resonance, atmosphere-controlled surface photovoltage spectroscopy, in situ diffuse reflectance infrared Fourier transform spectroscopy, etc., it is confirmed that the improved photoactivities are attributed to the downward shift of the valence band to obtain the strong driving force for water oxidation along with extension of the visible light response region by B doping and to the capture of photogenerated holes to enhance charge separation and then to accelerate the water oxidation process from the modified Ru-oxo clusters.
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Journal of Environmental Chemical Engineering
·
2022
·
IF 7.968
Chen Li,Tianyi Sun,Guohui Yi,Dashuai Zhang,Yan Zhang,Xiaoxue Lin,Jinrui Liu,Zaifeng Shi,Qiang Lin
A highly efficient visible light-driven photocatalytic membrane composed of Ag/CNQDs/g-C 3 N 4 and PVDF membranes was successfully prepared by vacuum filter crosslinking. This new type of photocatalytic membrane possessed both excellent photocatalytic degradation performance and photocatalytic self-cleaning properties. The Ag/CNQDs/g-C 3 N 4 photocatalyst coating amount of 10 mg had the highest photocatalytic degradation of norfloxacin (NOR), and the quasi-first-order kinetic constant ( k ) value was 0.0138 min −1 . Moreover, the mechanism of the photocatalytic reaction was also discussed. In addition, bovine serum albumin (BSA) as the simulated pollutant was applied to evaluate the self-cleaning property of the Ag/CNQDs/g-C 3 N 4 -PVDF composite membrane. After contamination with BSA, the water flux of the composite membrane decreased from 3880 L (m 2 h) −1 to 800 L (m 2 h) −1 . Then, the maximum pure water flux of the Ag/CNQDs/g-C 3 N 4 -PVDF photocatalytic composite membrane recovered 87% (3360 L (m 2 h) −1 ) within 90 min of visible light irradiation, indicating that the Ag/CNQDs/g-C 3 N 4 -PVDF photocatalytic composite membrane had excellent self-cleaning properties.
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ELECTROCHIMICA ACTA
·
2022
·
IF 7.336
Qianqing Wu,Zhenhui Li,Qianwei Liang,Rongkai Ye,Shuzhou Guo,Xiaobing Zeng,Jianqiang Hu,Aiqing Li
MicroRNAs (miRNAs) are considered as potential biomarkers for early diagnosis and prognostic assessment of diabetic nephropathy. In this work, an electrochemical biosensor for ultrasensitive detection of miRNA-377 was constructed based on MXene-Au nanocomposites and G-quadruplex nano-amplification strategy. As a promising nanocarrier, taking advantage of leveraging synergistic effects between Au nanoparticles (AuNPs) and MXene nanosheet, MXene-Au nanocomposites exhibited excellent electronic conductivity and provided massive active sites for DNA capture probe immobilization by Au-S bonds. AuNPs modified with Guanine-rich sequence DNA detection probes were designed as signal amplification nano-labels. Specifically, by inducing the transition of Guanine-rich detection probes to G-quadruplex, the strong affinity interaction between methylene blue and G-quadruplex could not only reflect trace concentration information of miRNA-377, but also lead to the further enhancement of electrochemical signal (2.7-fold). As a result, this newly designed biosensor exhibited superior sensing performance with a wide linear range from 10 aM to 100 pM and the limit of detection was as low as 1.35 aM. Compared with biosensors based on other nanocomposites and reported miRNA-377 biosensors, the proposed sensing platform did not require any thermal cycling or reverse transcription process, meeting the miRNA sensing requirements of convenient, sensitive, specific and stable. Furthermore, the as-constructed biosensor also displayed good selectivity, which was applied to accurate detection of miRNA-377 in human serum samples with satisfactory sensitivity, suggesting the biosensor system has promising applications in biological researches and early clinical diagnosis for diabetic nephropathy.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Desen Zhou,Jun Zhang,Zhenxing Jin,Tingmin Di,Tielin Wang
Photocatalytic CO 2 reduction has been considered as a potential way to solve the energy problem and the greenhouse effect. In this work, layered g-C 3 N 4 /rGO/NiAl-LDHs heterojunctions were prepared by using a hydrothermal method, the optimized composite exhibited enhanced photocatalytic CO 2 reduction to CO (2.6 μmol h −1 g −1 ) and CH 4 (20 μmol h −1 g −1 ) activity, which was 3.7 and 14.2 times higher than that of pure g-C 3 N 4 , respectively. According to the experimental and density functional theory calculation (DFT) results, it is believed that with the large contact interface and excellent electron mobility rGO could act as an electron transfer bridge to facilitate the rapid charge migration and separation between g-C 3 N 4 and NiAl-LDHs. Thus, driven by the internal electric field, interfacial band edge bending, as well as the type II heterostructure, the activity of g-C 3 N 4 /rGO/NiAl-LDHs could be greatly enhanced. This work provides a possible way to rational design and fabrication of rGO-assisted composite systems with type II, Schottky, S-scheme, P-N and other heterojunctions.
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CHEMOSPHERE
·
2022
·
IF 8.943
Xiaohui Zhan,Yue Zhao,Yanping Sun,Chen Lei,He Wang,Huixiang Shi
In this study, with thiourea and 3-aminopyridazine as precursors, the graphite-phase carbon nitride (ACN-x) with nitrogen defects and sponge structure is prepared via the introduction of the benzene-like ring structure of pyridazine replacing a “melem” group through hydrothermal procedure combined with calcination. It is made possible by the attraction of three hydrogen bond receptors for 3-aminopyrazine to lone pair electrons on the “melem” molecule. The remarkable extensively photocatalytic activity can be attributed to three effects of the introduction of 3-aminopyridazine: (i)formation of nitrogen defects between adjacent tri-s-triazine groups; (ii)formation of effective charge transfer channels within the tri-s-triazine group; (iii)the spongy structure exposed abundant amino groups(-NH 3 ) at edge sites, combining with the internal amino group and as hole stabilizer to prolong the excited state life of photocatalyst. The photogenerated carrier migration and separation efficiency improved effectively through the tuning synergy. As a result, ACN-x exhibits excellent photocatalytic activity, with hydrogen production efficiency of up to 11331.74 μmol g −1 h −1 , which is approximately 94.5 times that of the pristine g-C 3 N 4 (119.88 μmol g −1 h −1 ). The degradation constants of TC and RhB are 0.0498min −1 and 0.129min −1 , which are 3.32 and 6.35 times of the pristine g-C 3 N 4 , respectively. The TC degradation in different initial concentrations, pH, dissolved organic matter concentrations, and water sources is conducted to prove the environmental adaptability of the ACN-x system. The mechanism of the system indicates that ·O 2 − plays an important role, and the ·OH and h + play a minor role in the TC photocatalytic degradation . Finally, the TC degradation possible pathway is proposed.
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Journal of Environmental Chemical Engineering
·
2022
·
IF 7.968
Ling-Hui Kong,Yan Wu,Rong-Fang Shen,Wen-Jie Zhang,Zhen-Yue Dong,Wen-Ting Ge,Xiao-Jing Guo,Xi Yan,Yan Chen,Wan-Zhong Lang
Herein, N-doped porous carbon (NPC) and g-C 3 N 4 were combined as peroxymonosulfate (PMS) activator, showing excellent catalytic performance for the degradation of rhodamine B (RhB), methyl orange (MO) and tetracycline (TC). A synergistic effect was proved to exist between NPC and g-C 3 N 4 in the as-prepared catalyst (g-C 3 N 4 @NPC). The radical quenching study, electron paramagnetic resonance (EPR) measurement, LSV measurements and electrochemical EIS were performed to examine RhB degradation mechanism. The main degradation intermediates of RhB were identified by LC-MS, and the possible degradation pathways were proposed. The effects of pH, temperature and natural substances on RhB degradation were investigated. Cycling experiments and the degradation of RhB in tap water and river water showed that the g-C 3 N 4 @NPC/PMS system had practical prospects for environmental remediation.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Wenyuan Ye,Jinjie Chen,Na Kong,Qingyuan Fang,Mingqiu Hong,Yuxiang Sun,Yifan Li,Patricia Luis,Bart Van der Bruggen,Shengqiong Fang,Shuaifei Zhao,Jiuyang Lin,Shungui Zhou
Conventional membrane processes, e.g., microfiltration and ultrafiltration, suffer from severe permeation flux decline and fouling during the oily wastewater treatment. The superhydrophilic surface decoration provides an important and effective strategy to address this challenge. Herein, a surperhydrophilic/underwater superoleophobic nanocomposite surface with the photocatalytic properties was constructed via one-step facile vacuum-assisted filtration of a g-C 3 N 4 nanosheet/SiO 2 nanoparticle dispersion onto a microfiltration membrane substrate. Specifically, with the intercalation of 20 mg∙L −1 SiO 2 nanoparticles into the g-C 3 N 4 nanosheets, the g-C 3 N 4 /SiO 2 composite membrane showed the superhydrophilic/underwater superoleophobic properties with an underwater oil contact angle of 170.0 ± 0.3°. Such a g-C 3 N 4 /SiO 2 composite membrane yielded a permeation flux of >1290 LMH·bar −1 with an oil rejection of >99.91% during the vacuum filtration of oil-in-water emulsions. The g-C 3 N 4 /SiO 2 composite membrane significantly outperformed the pristine microfiltration substrate that had severe fouling caused by oil blockage. Additionally, the g-C 3 N 4 /SiO 2 composite membrane not only effectively retained the E. coli bacteria through size exclusion effect, but also promoted the inactivation of bacteria via visible-light photocatalysis. Therefore, our membrane has a great promise in practical oily wastewater treatment due to its excellent separation performance and biofouling resistance.
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ACS Omega
·
2022
·
IF 4.132
Lina Zhang,Ying Zhang,Baikang Zhu,Jian Guo,Dongguang Wang,Zhongqi Cao,Lihui Chen,Luhui Wang,Chunyang Zhai,Hengcong Tao
Electrochemical CO2 reduction has been acknowledged as a hopeful tactic to alleviate environmental and global energy crises. Herein, we designed an Fe@C/g-C3N4 heterogeneous nanocomposite material by a simple one-pot method, which we applied to the electrocatalytic CO2 reduction reaction (ECR). Our optimized 20 mg-Fe@C/g-C3N4-1100 catalyst displays excellent performance for the ECR and a maximum Faradaic efficiency (FE) of 88% with a low overpotential of −0.38 V vs. RHE. The Tafel slope reveals that the first electron transfer, which involves a surface-adsorbed *COOH intermediate, is the rate-determining step for 20 mg-Fe@C/C3N4-1100 during the ECR. More precisely, the coordinating capability of the g-C3N4 framework and Fe@C species as a highly active site promote the intermediate product transmission. These results indicate that the combination of temperature adjustment and precursor optimization is key to facilitating the ECR of an iron-based catalyst.
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Materials Today Chemistry
·
2022
·
IF 7.613
Y. Chen,M. Yang,Y. Jia,P. Yan,F. Chen,J. Qian,L. Xu,H. Li
Photoelectrochemical (PEC) aptasensor based on photoactive species with remarkable and stable PEC response is a rising analytical method to implement highly efficient and sensitive detection of residual antibiotics in the field of food. Herein, NiS 2 /NiFe-layered double/graphitic carbon nitride (NiS 2 /NiFe LDH/g-C 3 N 4 ) ternary heterostructure designed by the surface vulcanization of flower-like NiFe LDH/g-C 3 N 4 was used for developing a label-free PEC aptasensing platform to detect enrofloxacin (ENR). The introduction of NiS 2 with narrow bandgap can strengthen the light harvesting of solar energy, producing large amounts of photoinduced carriers. NiS 2 as the electrons conduction bridge further accelerates the transmission efficiency of electrons in contrast to binary heterojunction, endowing ternary heterostructure with superior photocurrent signal. A label-free PEC aptasensor detected ENR with an amplified detection signal because of the oxidation of ENR molecules by photoinduced holes. This PEC aptasensing platform of ENR manifested a wide detection range from 3.6 × 10 −7 to 30 ng/mL with a low detection limit of 1.2 × 10 −7 ng/mL as well as can provide a sensitive and stable analysis with feasible application to monitor milk and honey samples. This design can open the utilization of ternary heterostructure by surface vulcanization to improve the sensitivity of PEC aptasensing platform for monitoring environmental pollutants.
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JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
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2022
·
IF 6.76
Hongyu Zhang,Ling Chen,Baogang Xu,Ping Yang
The strong band-to-band visible light absorption obtained by changing the bandgap of photocatalysts is desirable but challenging for TiO 2 . In this paper, a mechanochemical pre-reaction and subsequent heat-treatment process were used to create TiO 2 /g-C 3 N 4 heterojunctions. Acid-treated H 2 Ti 3 O 7 nanobelts and superior thin g-C 3 N 4 nanosheets (CN) were ground evenly and further heat-treated to grow rhombic TiO 2 in situ on the nanosheets. The heterojunctions exhibited a band gap with the absorption in visible light region. Heterojunction formation effective tunes the surface and electronic structures of the composite, resulting in significant decrease of bandgap. g-C 3 N 4 -based heterojunctions (5TCN) exhibited excellent H 2 generation (4991 μmol/g/h) and NO removal. In contrast, a TiO 2 -based composite (95TCN) revealed efficient photo reduction of Cr(Ⅵ) which was 2 times of that of TiO 2 sample and 22 times of that of CN. The photochemical reaction mechanism of TiO 2 and g-C 3 N 4 -based composites was discussed with the ratio of TiO 2 and g-C 3 N 4 . The excellent performance is ascribed to single crystal rhombic TiO 2 nanoparticles grown in situ on g-C 3 N 4 to form well-developed heterojunctions which accelerate the carrier transfer. These results inspire the electronic structure engineering of photocatalysts to improve visible light absorption and provide a magic strategy for excellent photochemical activities.
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CHEMBIOCHEM
·
2022
·Vol. 23
·期 11
·e202200179
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IF 3.461
Shiyi Song,Yingying Jiang,Ruidong Chen,Wencheng Su,Weinan Liang,Dameng Yang,Jincheng Li,Wuyuan Zhang,Shushan Gao,Bo Yuan,Ge Qu,Zhoutong Sun
Graphical Deacetoxycephalosporin C synthase (DAOCS) requires 2-oxoglutarate (2OG) as a co-substrate to catalyze the conversion of penicillin G to phenylacetyl-7-aminodeacetoxycephalosporin acid (G-7-ADCA). Catalase and L-GOX were introduced into the catalytic process of ring expansion to construct a 2OG production module to form a three-enzyme co-expression system, so as to realize the conversion of penicillin G to G-7-ADCA in vivo . Deacetoxycephalosporin C synthase (DAOCS) catalyzes the transformation of penicillin G to phenylacetyl-7-aminodeacetoxycephalosporanic acid (G-7-ADCA) for which it depends on 2-oxoglutarate (2OG) as co-substrate. However, the low activity of DAOCS and the expense of 2OG restricts its practical applications in the production of G-7-ADCA. Herein, a rational design campaign was performed on a DAOCS from Streptomyces clavuligerus (scDAOCS) in the quest to construct novel expandases. The resulting mutants showed 25∼58 % increase in activity compared to the template. The dominant DAOCS variants were then embedded into a three-enzyme co-expression system, consisting of a catalase and an L-glutamic oxidase for the generation of 2OG, to convert penicillin G to G-7-ADCA in E. coli . The engineered whole-cell enzyme cascade was applied to an up-scaled reaction, exhibiting a yield of G-7-ADCA up to 39.21 mM (14.6 g ⋅ L −1 ) with a conversion of 78.42 mol %. This work highlights the potential of the integrated whole-cell system that may inspire further research on green and efficient production of 7-ADCA.
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RSC Advances
·
2022
·Vol. 12
·期 17
·10258-10266
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IF 4.036
Jing Liu,Jinxiao Zheng,Guichu Yue,Huaike Li,Zhaoyue Liu,Yong Zhao,Nü Wang,Chenghua Sun,Zhimin Cui
TiO2/g-C3N4 composite photocatalysts with various merits, including low-cost, non-toxic, and environment friendliness, have potential application for producing clean energy and removing organic pollutants to deal with the global energy shortage and environmental contamination. Coating a continuous g-C3N4 layer on TiO2 fibers to form a core/shell structure that could improve the separation and transit efficiency of photo-induced carriers in photocatalytic reactions is still a challenge. In this work, porous TiO2 (P-TiO2)@g-C3N4 fibers were prepared by a hard template-assisted electrospinning method together with the g-C3N4 precursor in an immersing and calcination process. The continuous g-C3N4 layer was fully packed around the P-TiO2 fibers tightly to form a TiO2@g-C3N4 core/shell composite with a strong TiO2/g-C3N4 heterojunction, which greatly enhanced the separation efficiency of photo-induced electrons and holes. Moreover, the great length–diameter ratio configuration of the fiber catalyst was favorable for the recycling of the catalyst. The P-TiO2@g-C3N4 core/shell composite exhibited a significantly enhanced photocatalytic performance both in H2 generation and dye degradation reactions under visible light irradiation, owing to the specific P-TiO2@g-C3N4 core/shell structure and the high-quality TiO2/g-C3N4 heterojunction in the photocatalyst. This work offers a promising strategy to produce photocatalysts with high efficiency in visible light through a rational structure design.
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