APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
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IF 20.2
Tao Shan,Sunzai Ke,Xin Yang,Xuhui Yang,Bo Weng,Lijuan Shen,Min-Quan Yang
Photocatalytic selective oxidation of aromatic hydrocarbons plays an important role in the production of value-added chemicals. A key step in this process is the activation of C(sp 3 )-H bond by photogenerated holes. However, the inadequate hole generation and lack of surface adsorption-activation sites severely hinders the improvement in photocatalytic C-H bond oxidation. In particular, the random charge migration to the surface impedes the effective capture of holes by surface active sites to dissociate the C(sp 3 )-H bond. Here, we design and fabricate a Co 3 O 4 /Cs 3 Sb 2 Br 9 p-n heterojunction that effectively addresses these challenges. The p-n heterojunction forms strong built-in electric fields (BEF) facilitating spatial charge separation. Holes are accumulated on Co 3 O 4 , while electrons are accumulated on Cs 3 Sb 2 Br 9 , thereby offering abundant active holes and electrons. Moreover, Co 3 O 4 shows stronger adsorption and activation capacity for the C(sp³)-H bond, enabling the C(sp 3 )-H bond dissociation with low reaction energy barrier. Consequently, the holes are directionally extracted from photoactive Cs 3 Sb 2 Br 9 to catalytically active Co 3 O 4 under visible light irradiation, thereby accelerating the toluene oxidation. The optimized 5 % Co 3 O 4 /Cs 3 Sb 2 Br 9 exhibits a benzyl aldehyde (BAD) evolution rate of 5044 μmol g −1 h −1 and a benzyl alcohol (BA) production rate of 1820 μmol g −1 h −1 , which are 12 and 17 times higher than that of blank Cs 3 Sb 2 Br 9 , respectively.
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ACS Catalysis
·
2025
·
IF 13.1
Tingting Xiao,Jingrong Li,Jian Li,Qihang Gong,Peikai Luo,Xinluona Su,Haiyang Cheng,Chao Zhang,Fengyu Zhao
The hydrogenolysis of cellulose-derived 5-hydroxymethylfurfural is essential for the production of fuels and chemicals from biomass. Herein, we fabricated a phosphorus-doped Pd/P-TiO2 catalyst for the hydrodeoxygenation of 5-hydroxymethylfurfural to 2,5-dimethylfuran. A large number of defects and electron-deficient Ti4+ sites (dTi4+) were formed by doping phosphorus into the TiO2 support, which could promote hydrogen spillover and reactant adsorption. Moreover, the spilled active hydrogen induced the formation of P–O(H)-dTi4+, which acted as a “Brønsted acidic site” to promote the activation of C–O bonds. Consequently, the Pd/P-TiO2 catalyst exhibited superb activity for the hydrodeoxygenation of 5-hydroxymethylfurfural to 2,5-dimethylfuran at mild conditions of 150 °C under 1 MPa H2.
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CHEMICAL ENGINEERING JOURNAL
·
2024
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IF 13.3
Xiao Zhang,Menglin Zhang,Xinyuan Li,Baoping Xin,Jie Hao,Jinying Li,Hansheng Li,Dongxiang Zhang,Zijie Wu,Xiyan Xu,Jiatao Zhang
The risk of radionuclide leakage always threats ecological security and human health, making the recovery of uranium from nuclear wastewater a meaningful and urgent issue. However, the low-cost and efficient capture of uranium remains a challenge at present. In this study, a homemade photocatalyst of iron coordinated graphitic carbon nitride (g-C 3 N 4 ) co-doped with phosphorus and oxygen (OPFCN), which was facilely synthesized through a novel one-step thermal polymerization method, exhibited superior photoelectric efficiency and photocatalytic activity towards the photo-reductive capture of uranium(VI). The simultaneous Fe coordination and P/O co-doping in framework of g-C 3 N 4 played a synergistic effect in charge reconstruction, in which electrons migration driven by coordinated Fe and lone electron pairs delocalization from doped P/O enormously increased electron density and enhanced charge transfer, thus effectively promoting the separation of photogenerated charge carriers. The specific surface area, pore volume and average pore size of OPFCN reached 70.2 m 2 ·g −1 , 0.157 cm 3 ·g −1 and 7.78 nm, respectively, exhibiting a trend increasingly beneficial for photocatalytic adsorption and mass transfer with successive introduction of Fe, P and O into original g-C 3 N 4 . With the simultaneous introduction of Fe, P and O, the optical absorption edge underwent a significant redshift and fluorescence emission intensity dropped by 75 % compared to that of CN, demonstrating the enhanced visible light capturing ability and significantly inhibited recombination of photogenerated charge carriers in OPFCN. As a result, a uranium capture rate of over 98 % was achieved with catalyst dosage of only 5:1 at pH 5 with OPFCN, demonstrating its competitive photo-reductive activity towards uranium(VI) uptake compared with previously reported g-C 3 N 4 -based photocatalysts. Meanwhile, OPFCN exhibited remarkable reusability and stability with even over 65 % uranium recovery rate and almost unchanged peak patterns in XRD and FT-IR in fifth reuse recycle. Additionally, it was demonstrated that e − and O 2 •− were the direct active species to realize the photoreduction of uranium(VI) over OPFCN, in which e − played the dominant role. The modification method of simultaneous Fe coordination and P/O co-doping would be expected to effectively promote the utilization of g-C 3 N 4 -based photocatalysts towards photo-reductive recovery of uranium(VI) from radioactive wastewater.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2024
·
IF 8.1
Qihang He,Lei Wang,Feng Xiao,Rong Su,Yu Jiang,Lichuan Chen,Zeyi Wang,Bin Jia,Ping He,Chao Chen,Yali Zeng,Yun Zhou,Bin Tang
The design of advanced noble-metal-free electrocatalysts with high activity and good stability for the hydrogen evolution process (HER) is both appealing and challenging. Herein, cauliflower-like Co–B–P nanoparticles anchored on multi-layered g-C 3 N 4 nanosheets (Co–B–P/g-C 3 N 4 ) are fabricated by a facile electroless deposition method at room temperature . The effect of P/B ratios on electrocatalytic performance of ternary Co–B–P/g-C 3 N 4 catalysts for HER is fully investigated in 1.0 M KOH solution. Due to both the synergetic effect among P, B and Co, and the support of multi-layered g-C 3 N 4 nanosheets , ternary Co–B–P/g-C 3 N 4 catalyst exhibits satisfactory electrocatalytic HER performances. The onset overpotential for the best ternary Co–B–P/g-C 3 N 4 catalyst is only 93 mV, whereas it is 173 mV for binary Co–B/g-C 3 N 4 catalyst. When current density achieves 10 mA cm −2 and 40 mA cm −2 , the required overpotentials for ternary Co–B–P/g-C 3 N 4 catalyst are 174 mV and 226 mV, respectively, which are much lower than those of binary Co–B/g-C 3 N 4 catalyst (261 mV and 327 mV). Furthermore, the stability test indicates that ternary Co–B–P/g-C 3 N 4 catalyst possesses a favorable long-term electrochemical stability under alkaline condition. The satisfactory electrocatalytic performances of as-prepared ternary Co–B–P/g-C 3 N 4 catalyst suggest that it is a promising candidate to substitute noble-metal based catalysts for HER.
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MICROCHIMICA ACTA
·
2024
·Vol. 191
·期 7
·1-11
·
IF 5.3
Li Huiru,Tian Yanbo,Tan Liju,Wang Na,Qiao Yu,Wang Jiangtao
A novel molecularly imprinted ratiometric fluorescent sensor CQDs@MIP/FITC@SiO 2 for the detection of p-nitroaniline (p-NA) was constructed through the mixture of CQDs@MIP and FITC@SiO 2 in the ratio of 1:1 ( V CQDs@MIP : V FITC@SiO₂ ). The polymers of CQDs@MIP and FITC@SiO 2 were prepared by sol-gel method and reversed-phase microemulsion method, respectively. CQDs@MIP was used as the auxiliary response signal and FITC@SiO 2 was used as the reference enhancement signal. The signal was measured at excitation/emission wavelengths of 365/438, 512 nm. The sensor showed good linearity in the concentration range 0.14–40.00 µM ( R 2 = 0.998) with a detection limit of 0.042 µM for p-NA. The color change of “blue-cyan-green” could be observed by the naked eye under 365 nm UV light, thus realizing the visual detection of p-NA. The sensor presented comparable results compared with high-performance liquid chromatography (HPLC) method for the detection of p-NA in hair dye paste and aqueous samples with recoveries of 96.8–103.7% and 95.8–104.4%, respectively. It was demonstrated that the constructed sensor possesses the advantages of simplicity, excellent selectivity, superior sensitivity, and outstanding stability. Graphical Abstract
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JOURNAL OF ETHNOPHARMACOLOGY
·
2025
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IF 5.4
Junying Li,Xiaoxiao Shan,Yu Gao,Haizhou Zhu,Hongyan Cheng,Chengjie Xing,Lele Zhou,Wenkang Tao,Yangyang Li,Baoqi Yin,Caiyun Zhang
Ethnopharmacological relevance Kai-Xin-San (KXS) has a significant effect therapeutic on Alzheimer's disease (AD) in clinical practice. According to the compatibility theory of traditional Chinese medicine, Acori Tatarinowii Rhizoma (ATR) serves as the guiding drug in the KXS formulation and is believed to enhance the bioavailability and brain tissue distribution of the other drugs. However, the mechanism underlying the “guiding medicine upwards” effect of ATR in KXS remains unexplored. Aim of the study The aim of this study is to investigate the role of ATR in the efficacy of KXS on amyloid precursor protein/presenilin 1 (APP/PS1) mice, as well as its impact on the brain tissue distribution of other active ingredients in the KXS formula, and to elucidate the mechanism of ATR's “guiding medicine upwards” effect in KXS. Materials and methods The pharmacodynamic effects of ATR in KXS were assessed through behavioral tests, immunohistochemical staining, and Nissl staining. Additionally, the levels of inflammatory factors, as well as the activities of malondialdehyde, superoxide dismutase, and acetylcholinesterase, were measured using enzyme-linked immunosorbent assay kits. Subsequently, the effect of ATR on the ultrastructure of the blood-brain barrier (BBB) in APP/PS1 mice was observed using transmission electron microscopy (TEM), and the pharmacodynamic components of KXS in cerebrospinal fluid were quantified by ultra-high-performance liquid chromatography-triple quadrupole mass spectrometry (UPLC-MS/MS). Furthermore, Western blot (WB) analysis was used to quantitatively assess the expression of tight junction proteins (Claudin-5, Occludin, and ZO-1) and transporters (OCT3, OATP2, P-gp, and MRP1) in the BBB. Finally, bEND.3 cells and astrocyte cells were co-cultured to validate the effect of ATR on KXS. The expressions of OCT3/OATP2 and P-gp/MRP1 in BBB cell model were determined by WB and the content of pharmacodynamic components in the lower chamber of the transwell were also analyzed by UPLC-MS/MS. Results Behavioral test results suggest that KXS significantly improved the learning and memory capacities of APP/PS1 mice compared to the ATR-free KXS group. Furthermore, KXS was more effective in reducing amyloid-β protein deposition in the brain and repairing damaged neurons in the CA1 and CA3 regions than ATR-free KXS. Notably, KXS significantly reversed the pathological biochemical indices compared to the ATR-free KXS group. These results indicate that ATR has a positive effect on the pharmacodynamics of KXS in treating AD. Most importantly, TEM results revealed that KXS repaired the damaged BBB in AD mice, and ATR contributed to the improvement of BBB integrity. Furthermore, KXS and ATR increased the expression levels of Claudin-5, Occludin, and ZO-1 proteins in AD mice. Meanwhile, the levels of ginsenoside Rg1, ginsenoside Rb1, and polygalaxanthone III in the cerebrospinal fluid of the KXS group were 1.47, 1.39, and 2.02 times higher than those in the ATR-free KXS group, respectively. WB results showed that ATR and KXS significantly upregulated the expression of OCT3/OATP2 uptake transporters and downregulated the expression of P-gp/MRP1 efflux transporters compared to ATR-free KXS. Concurrently, in vitro BBB cell experimental results suggest that ATR promoted the transport of ginsenoside Rg1, ginsenoside Rb1, and polygalaxanthone III across BBB cells in KXS, and the regulation of OCT3/OATP2 and P-gp/MRP1 expression was consistent with the in vivo trends observed in AD mice. Conclusions ATR plays a critical role in enhancing the efficacy of KXS in treating AD and facilitates the entry of other pharmacodynamic components into the brain. The mechanism underlying the “guiding medicine upwards” effect of ATR may involve the regulation of OCT3/OATP2 and P-gp/MRP1 transporters.
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Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Guang-En Yuan,Yan-Ge Ma,Kangning Huangfu,Yunbei Li,Xin Zhang,Fenglin Yang
Advanced oxidation processes based on the combination of zero-valent iron (ZVI) and S(IV) have been extensively investigated for oxidative degradation of organic pollutants, but little attention has been paid to their reducing capacities in the presence of oxygen. This work found bisulfite (BS) could greatly enhance the degradation of p-nitrophenol (PNP) by ZVI under oxic conditions and PNP was only reduced to p-aminophenol without further degradation. A combination of indirect reduction by superoxide radical (O 2 •– ) and direct reduction by ZVI was verified as the mechanism of PNP degradation. Highly oxidizing species, such as hydroxyl radical (HO • ) and sulfate radical (SO 4 •− ), were also produced in the ZVI/BS system under oxic conditions but did not contribute to pollutant degradation perhaps due to the rapid consumption by reducing substances like BS ions and the released Fe 2+ . BS concentration, ZVI dosage, initial solution pH and coexisting anions (CO 3 2– , PO 4 3– and Cl – ) affected the degradation of PNP. ZVI lost the reactivity after used for three times because of the production of goethite and lepidocrocite covered on its surface. This study will provide a new insight into degradation of organic pollutants in ZVI/BS system under oxic conditions.
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ORGANOMETALLICS
·
2024
·
IF 2.5
Hong Chen,Weiwei Zuo
Asymmetric transfer hydrogenation (ATH) of ketones is an efficient method for constructing chiral alcohols that are widely used in synthesizing various fine chemicals. Currently, most of the existing catalysts contain precious metals that are highly toxic and scarce, which limits industrial application and sustainability. Therefore, the development of catalysts based on earth-abundant and environmentally friendly 3d metals is an important research topic. We previously reported that amido-ene(amido)diphosphine Ni(II) catalysts exhibited promising reactivities. However, the enantioselectivity of the catalytic system was not satisfactory. Here, we report (primary amido)-ene(amido)Ni(II)diphosphine catalyst 2n containing a P-chirogenic substituted ferrocene moiety in the ligand backbone and its analogue (2m). 2n was used for ATHs of a range of ketones with improved enantioselectivity, affording secondary alcohols of the (S)-configuration with up to 98% enantiomeric excess (e.e.). Computational results indicated that in the reaction system of catalyst 2n, the (S)-configuration of the phosphine kept the (S)-planar chiral ferrocene moiety far from the reacting site in the transition state that produced the (S)-configured alcohol. This created space for the aryl ring of the substrate and the ene(amido) moiety of the catalyst to approach each other and form a strong π–π interaction that enhanced the enantioselectivity.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2024
·
IF 5.8
Jiahuan Cao,Yujia Wu,Yinghuan Fu,Yu Song,Guowen Wang,Hongchao Ma
Photocathodic protection is a promotion strategy for the corrosion protection of metallic materials, and the selection of photocathodic materials is a critical factor in improving the performance of photocathodic protection of metallic materials. Herein, a Ti-P-V-O composite semiconductor photoelectrode with an adjustable porous structure was prepared by the micro-arc oxidation (MAO) method using titanium alloy (TC 4 ) as the matrix and ammonium metavanadate (NH 4 VO 3 ) as the additive. The photogenerated open circuit potential, instantaneous photocurrent density response value, electrochemical impedance spectroscopy, and Tafel curve of as-prepared Ti-P-V-O photo-electrodes were measured after coupling with 304SS to clarify the cathodic protection effect for 304 stainless steel (304SS). It is found that the as-prepared Ti-P-V-O coating photoelectrode has a more negative open circuit potential, a more significant photocurrent density response, more effective interface carrier transport ability, lower resistance, lower compounding efficiency of photogenerated electron/hole pairs, and more negative conduction band level, as compared with that of TiO 2 coatings. Moreover, the optimized Ti-P-V-O photoelectrode (Ti-P-V-O&300 V) exhibited the maximum negative shift of the corrosion potential (410 mV vs. SCE) for coupling with 304 stainless steel. This work presents a new strategy for constructing an efficient coating photo-electrode for photocathodic protection of metallic materials.
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APPLIED SURFACE SCIENCE
·
2024
·
IF 6.3
Mei Dong,Wenjun Li,Liang Geng,Ruixue Huang,Yuan Liu,Hongli Han
Herein, CuCo 2 O 4 hollow porous nanospheres (HPN), nanosheets (NS), and nanowires (NW) were synthesized via solvothermal and calcination processes, and were used to construct efficient heterojunctions with Cd 0.5 Zn 0.5 S. Interestingly, the unique hollow porous structure exhibits enhanced light absorption, large pore diameter (12.57 nm), and strong hydrophilicity (10.05°). Photocatalytic results indicate that CuCo 2 O 4 HPN/Cd 0.5 Zn 0.5 S achieves the optimal hydrogen production rate, which is 5.4, 1.2, and 1.3 times than that of pure Cd 0.5 Zn 0.5 S, CuCo 2 O 4 NW/Cd 0.5 Zn 0.5 S and CuCo 2 O 4 NS/Cd 0.5 Zn 0.5 S, respectively. High-resolution TEM and theoretical calculations confirm that (311)/(111) facet junctions in CuCo 2 O 4 nanospheres form a work function difference (0.24 eV), which significantly facilitates charge transfer and separation. Mott-Schottky and Ultraviolet photoelectron spectroscopy analyses indicate that p-type CuCo 2 O 4 and n-type Cd 0.5 Zn 0.5 S have staggered energy levels and a distinct Fermi level difference (1.85 eV), which leads to rearrangement of the Fermi energy level and modulation of charge transfer pathway. The resulting energy band bending and built-in electric field promote charge transfer at the heterojunction interface more effectively. The synergistic mechanism of the facet junction and p-n junction finally achieves high-efficiency hydrogen production. This work provides new insights into how to construct efficient p-n heterojunction photocatalysts and presents the synergistic mechanism of facet junction and p-n junction.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Yue Sun,Chenrui Zhao,Jin Xu,Yazi Liu,Huan He,Feihu Mu,Wei Zhao,Dan Sun,Shaogui Yang,Cheng Sun
The construction of built-in electric field (BIEF) in heterojunction is an effective strategy to enhance solar-driven hydrogen (H 2 ) production by minimizing charge carrier recombination and improving transport kinetics. Herein, p-type ternary sulfide CuGaS 2 (CGS) and n-type g-C 3 N 4 nanosheets (CN) are integrated to construct a p-n heterojunction through a simple co-precipitation method for photocatalytic hydrogen evolution reaction (HER). In situ X-ray photoelectron spectroscopy (in situ XPS), in situ electron paramagnetic resonance (EPR) and density functional theory (DFT) calculations revealed that differences in Fermi levels and carrier concentrations between CGS and CN induce charge migration following an S-scheme mechanism, which aligned well with the intrinsic p-n junction field. The escalated BIEF effect enhances interfacial band bending, drives efficient charge separation, and promotes directional charge transfer. As a result, the optimized 20CN/CGS photocatalyst achieves a high H 2 evolution rate of 563 ± 5 μmol g cat −1 , approximately 3.3 times that of CGS. Additionally, the 20CN/CGS exhibits photothermal properties with further boosted HER rate of 732 ± 6 μmol g cat −1 at 35 °C, achieving a photothermal conversion efficiency (PCE) of 11 ± 2 %. This indicates its potential for exploitation of thermal heat from solar spectrum. This work provides a promising strategy for designing high-performance p-n heterojunction governed by S-scheme charge transfer to boost solar energy conversion.
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JOURNAL OF CELLULAR AND MOLECULAR MEDICINE
·
2025
·Vol. 29
·期 14
·e70659
·
IF 4.2
Hao Wang,Chi Zhang,Jinyue He,Zhuoen He,Shihua Yan,Yuan Zhang,Shiyin Huang,Yangtian Yan,Yuchi Chen,Zhiqiang Xian,Rong Hu,Yanjing Wang,Wei Xiao,Mingqing Wang
Skeletal muscle atrophy is a prevalent complication in chronic kidney disease (CKD), and its pathogenesis is closely related to inflammation and oxidative stress. P-Coumaric acid (PCA) is a phenolic acid with anti-inflammatory and antioxidant pharmacological actions. This research aims to investigate the effect of PCA on CKD-induced muscle atrophy and its underlying mechanism. In our study, in vivo and in vitro models were established by using 5/6 nephrectomized rats and LPS-induced C2C12 myoblasts. The experimental results showed that PCA ameliorated kidney injury in CKD rats and increased skeletal muscle weight and the cross-sectional area of muscle fibres. In both CKD rats and LPS-induced C2C12 myoblasts, PCA also exhibited anti-inflammatory and antioxidant effects, reduced the levels of pro-inflammatory cytokines and enhanced the activity of antioxidant enzymes. Network pharmacology studies have identified 165 common targets between PCA and skeletal muscle atrophy. Furthermore, the experimental results also demonstrated that PCA decreased the expression of TLR4, MyD88, NF-κB p65, MurF1 and MAFbx at both the protein and mRNA levels. Additionally, in vitro experiments showed that the use of TLR4 agonists could reverse the muscle-protective effect of PCA. In summary, this study illustrated that PCA ameliorated skeletal muscle atrophy in CKD rats by inhibiting the TLR4/MyD88/NF-κB pathway.
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