ACS Omega
·
2023
·
IF 4.1
Dandan Cheng,Xin Han,Jiawen Zou,Zhenyu Li,Meiru Wang,Yuqing Liu,Kexuan Wang,Yan Li
We have reported the synthesis of epitope-imprinted mesoporous silica (EIMS) with an average pore size of 6.2 nm, which is similar to the geometrical size of the target protein, cytochrome C (Cyt c, 2.6 × 3.2 × 3.3 nm3), showing great recognition and large-scale adsorption performance. The characteristic fragment of Cyt c was used as a template and docked onto the surface of C16MIMCl micelles via multiple interactions. Nitrogen adsorption–desorption and transmission electron microscopy confirmed the successful preparation of EIMS. Due to the ordered pore structure, larger pore size, and high specific surface area, the prepared EIMS show superior specificity (IF = 3.8), excellent selectivity toward Cyt c, high adsorption capacity (249.6 mg g–1), and fast adsorption equilibrium (10 min). This study demonstrates the potential application of EIMS with a controllable pore size for high-effective and large-scale separation of Cyt c, providing a new approach for effective biomacromolecular recognition.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Weirui Chen,Siyou Fu,Xukai Li,Jing Wang,Xunan Ning,Liying Bin,Ping Li,Bing Tang,Laisheng Li
Photocatalytic ozonation (PCO) was a novel water treatment method, but the low photo-generated electron ( e - ) utilization and ambiguous ROS formation mechanism restrained its performance. Herein, C vacancy and F co-decorated g-C 3 N 4 (FCN_Cv) was designed to accelerate the PCO performance with sodium p -perfluorinated nonoxybenzenesulfonate (OBS) acting as model pollutant. Comparative characterizations revealed that FCN_Cv remained the inherent structure of g-C 3 N 4 (BCN), and had an enhanced conduction band potential, narrower band gap and longer e - lifetime. FCN_Cv exhibited the greater activity over BCN, with 99.3 % OBS removal in 30 min but only 78.3 % for BCN during PCO process. •OH was the main ROS for degrading OBS. The greater •OH yield was obtained by FCN_Cv PCO process because of the increase of e - utilization. On one hand, the two electrons reduction of O 2 into H 2 O 2 on FCN_Cv was accelerated, which triggered the peroxone reaction between photogenerated-H 2 O 2 and O 3 . On the other hand, the direct one electron reduction of O 3 by e - also accounted for •OH generation. 17 kinds of intermediates were detected and the OBS degradation routes were inferred, which was involved with hydroxylation, C-O cleavage and aromatic ring opening reactions. Overall, this study demonstrated the feasibility of decorating F element and C vacancy on g-C 3 N 4 in enhancing e - utilization and •OH generation during PCO process as well as deepened the understanding of fate of OBS in PCO process.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2022
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IF 5.518
Jun Yu,Bin Hu,Pengfei Nie,Xiaohong Shang,Boshuang Zhang,Zhaoyu Tang,Jianmao Yang,Jianyun Liu
Norfloxacin (NX), as one of the most widely used antibiotics, is becoming a potential pollutant in water. Here, the cobalt-decorated nitrogen-rich carbon material containing abundant carbon nanotubes (Co@C-NCNTs) was synthesized by pyrolysis of the Co,Zn bimetal organic frameworks (Co,Zn-MOF). The introduction of Zn led to the formation of abundant CNTs with high aspect ratio and high N-doping in the carbon metrix. The obtained Co@C-NCNTs catalyst was applied to boost non-radical catalysis of peroxymonosulfate for NX degradation with high efficiency. The release of cobalt was greatly inhibited by Co-N interaction and carbon layer protection. The CNTs amount in Co@C-NCNTs and its catalytic activity were tunable with the Zn/Co ratio. At the optimal Zn/Co ratio, the derived Co@C-NCNTs delivered 92% removal of NX in 30 min, significantly higher than the single Co-MOF based catalyst. Free radical quenching experiments and electron paramagnetic resonance demonstrated the singlet 1 O 2 -dominated degradation process of NX accompanied by the •OH and S O 4 − effect. The electrochemical characterization verified that the electron transfer in the PMS system is greatly enhanced due to the presence of Co@C-NCNTs.
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Catalysis Science & Technology
·
2023
·Vol. 14
·期 1
·137-144
·
IF 5
Zhibing Chen,Yali Lv,Xintai Chen,Xiaoling Mou,Jingwei Li,Li Yan,Ronghe Lin,Yunjie Ding
The development of non-precious metal catalysts to replace Pd-based industrial catalysts for 1,3-butadiene hydrogenation is highly desired. However, the cheap transition metal-based candidates developed to date, including Ni, Cu, Co, and Fe, show lower activity than precious metal catalysts, and typically suffer from deactivation due to coke deposition. In this contribution, an InNi3 alloy catalyst is designed via depletion of the layers of a carbon-capped interstitial compound InNi3C0.5 by two different approaches, hydrogenation and air oxidation, under varying conditions. The carbon depletion processes are followed by combined techniques to determine the full structural and compositional evolution processes, and the resulting catalysts are thoroughly characterized and evaluated for the selective hydrogenation of 1,3-butadiene. The InNi3 alloy serves as a coke-resistant low-temperature catalyst for 1,3-butadiene hydrogenation, achieving >94% total butene selectivity at >96% conversion at a mild temperature of 318 K. Post characterization of the catalyst after long-term testing verifies the structural robustness and excludes the accumulation of carbonaceous deposits, thus confirming the InNi3 alloy as a novel and promising system for selective hydrogenations.
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Materials
·
2023
·Vol. 16
·期 22
·7155
·
IF 3.4
Haozhi Duan,Dehai Meng,Shuxia Yuan
Solution combustion synthesis (SCS) is considered as an efficient and energy-saving method for preparing LiFePO4/C composite material with the nanostructure (Nano-LiFePO4/C). In this study, Nano-LiFePO4/C cathode material was prepared using SCS using a cost-effective combination of urea and sorbitol as mixed fuels. The effect of mixed fuels on combustion behavior and microstructure as well as on electrochemical performance was studied using XRD, BET, SEM, TEM, and electrochemical characterization methods. Multiple characterization results indicated that the maximum temperature (Tm) and particle size were influenced by the usage of urea and sorbitol. The sample derived under optimum conditions exhibits a mesoporous nanostructure with a large surface specific area and attractive electrochemical performance with a discharge capacity of 153.5 mAh/g at 0.1 C, which shows strong potential for commercial applications in the future.Keywords:LiFePO4;cathode materials;solution combustion synthesis;electrochemical performance;mixed fuels
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JOURNAL OF NANOPARTICLE RESEARCH
·
2023
·Vol. 25
·期 11
·1-12
·
IF 2.5
Li Fangyuan,Yao Niu,Yuan Huiyu,Cui Junyan,Jia Quanli
The redox properties of electrode materials play a vital role in electrochemical performance. Fabrication of electrode materials with multiple oxidation species is highly desired for ultrasensitive glucose sensing. Herein, multivalent Cu/Cu 2 O/CuO/C (Cu/C) nanocomposites were successfully prepared for non-enzymatic glucose sensing by in situ pyrolysis of Cu metal-organic framework (Cu 3 (BTC) 2 ·3H 2 O, Cu-BTC) at a critical temperature. Structure characterizations showed that the nanocomposites maintained the original morphology of Cu-BTC crystals and exhibited mesoporous structures. Meanwhile, multiple Cu species containing Cu, Cu 2 O and CuO were generated simultaneously, which were tightly pinned on the ligand-derived carbon layers. Thus, under the synergistic effect of multivalent Cu species, mesoporous structure and intense interface contact, the sensing platforms based on Cu/C nanocomposites exhibited good glucose detection performance with a wide linear range of 0.005-2.0 mM, ultrasensitivity of 147.65 μA mM -1 cm -2 , low detection limit of 6.31 μM (S/N = 3), and favorable anti-interference properties and stability. Especially, the Cu/C sensing platform showed excellent recoveries of glucose when used to monitor glucose in real sample of honey. The good electrochemical activities of Cu/C nanocomposites render them promising candidates for sensors and other applications. Graphical abstract
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BIOORGANIC & MEDICINAL CHEMISTRY
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2018
·
IF 2.881
Ping Zhou,Gang Chen,Minqi Gao,Jiaquan Wu
Osimertinib has been approved as a first-line treatment for non-small-cell lung cancer (NSCLC) patients whose tumor carries EGFR activation and / or resistant mutations. To mitigate Osimertinib’s toxicity caused by AZ5104, the N-demethylation metabolite of Osimertinib, we designed and synthesized a series of Osimertinib analogs with different headpieces. In vitro and in vivo analysis rendered a potential clinical candidate C-005 which had pyrrolo-pyridine headpiece. Biochemically, C-005 and its main human hepatocyte metabolite showed over 30 fold selectivity of L858R/T790M mutant EGFR over WT EGFR. Such selectivity profile was retained at cellular level. In general, C-005 is 2-14 fold more selective than Osimertinib in a panel of WT EGFR cancer cell lines. Furthermore, C-005 demonstrated robust antitumor efficacy and good tolerability in NCI-H1975, PC-9 and HCC827 xenograft mouse models, making it a potential candidate for human test in clinical.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Dafeng Zhang,Dong Zhang,Shikai Wang,Hengshuai Li,Junchang Liu,Xipeng Pu,Peixian Chen,Ran Qin,Haiquan Hu,Peiqing Cai
Suppressing the electron-hole recombination rate of catalyst legitimately is one of the effective strategies to improve photocatalytic hydrogen evolution . Herein, carbon-coated metal oxide , ZnFe 2 O 4 @C (ZFO@C), nanoparticles were synthesized and employed to couple with quadrupedal Cd 0.9 Zn 0.1 S (CZS) via an ordinary ultrasonic self-assembly method combined with calcination to form a novel ZFO@C/CZS catalyst with step-scheme (S-scheme) heterojunction . The photocatalytic hydrogen evolution reaction (HER) was conducted to verify the enhanced photoactivity of ZFO@C/CZS. The optimal ZFO@C/CZS exhibits an extraordinary photocatalytic HER rate of 111.3 ± 0.9 mmol g -1 h −1 under visible-light irradiation, corresponding to an apparent quantum efficiency as high as (76.2 ± 0.9)% at 450 nm. Additionally, the as-synthesized ZFO@C/CZS composite exhibits high stability and recyclability. The excellent photocatalytic hydrogen evolution performance should arise from the formed S-scheme heterojunction and the unique ZFO@C core–shell structure, which inhibit electron hole recombination as well as provide more reactive sites. The pathway of S-scheme charge transfer was validated through density functional theory calculations and electrochemical measurements. This work provides a rational strategy for the synthesis of unique magnetic S-scheme heterojunction photocatalysts for water splitting under visible light irradiation.
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MATERIALS CHEMISTRY AND PHYSICS
·
2023
·
IF 4.6
Hua Ma,Xiuwen Wu,Xiuli Fu,Zhijian Peng
Industrial-scale water splitting processes will require economical and efficient electrocatalyst materials. Many oxygen evolution electrocatalysts prepared with non-precious metals have been reported. However, transition metal-based nanomaterials experience unavoidable aggregation and low stability in corrosion environments, which substantially reduces their catalytic performance. Herein, we successfully used a simple electrospinning technique followed by carbonation to synthesize a porous B-doped carbon fiber electrocatalyst with embedded B-doped FeNi alloy nanoparticles . To prepare the optimal catalyst sample, 1.05 g PAN, 5.0 mmol H 3 BO 3 , 2.5 mmol Fe(NO 3 ) 3 , and 2.5 mmol Ni(NO 3 ) 2 were used as precursors. The electrospun pristine fibers were annealed for 1 h at 800 ° C in argon. Its overpotential for oxygen evolution at a current density of 10 mA cm −2 was only 231 mV, and a 60.99 mV·dec −1 Tafel slope was achieved. At this current density, this catalyst exhibits good performance for over 24 h or for more than 1000 CV cycles. This is due to the doping of non-metallic B atoms into the alloy nanoparticles , as well as the support and protection on them by carbon nanofibers . Insight This research provides a more thorough understanding of the preparation and practical application of low-cost and high-efficiency transitional metal alloy based water splitting catalysts.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Yuan Li,Miao-Ying Chen,Bang-An Lu,Hao-Ran Wu,Jia-Nan Zhang
Although the Mn-N-C catalyst has low toxicity and high durability, its intense pH-dependent ORR activity is perplexing and prevents its commercial use in PEMFCs. Herein, we have developed a novel understanding of the role of hydrogen peroxide in the pH-dependent activity and stability of Mn-N-C catalysts. Instead of nitrogen protonation, the strong pH effects of ORR activity are caused by the much faster kinetics of the H 2 O 2 reduction reaction in alkaline medium than in acid, due to the lower dissociation energy of the HO-OH bond in alkaline environment. Regarding durability, the deactivation induced by H 2 O 2 demonstrates a strong pH dependence, primarily due to the differing intensities of reactive oxygen species at different pH values. Correspondingly, isopropanol effectively reduces Fenton reagents and increases the acid resistance of Mn-N-C sites. The present research provides a mechanistic understanding of pH effects and paves the way for the creation of more efficient catalysts.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2023
·
IF 6.2
Shushu Li,Maozheng Li,Ruocheng Shen,Zhenzhen Liu,Xiaoyan Lv,Jing Su,Hongxiang Kuai,Yanxuan Wen
The emergence of layered structure materials has positioned itself as a focal point in the progress of potassium-ion battery (KIBs) cathode materials , as it faces challenges concerning cycling-induced structural stability. In this particular investigation, the successful synthesis of a carbon-coated polyanionic layered composite denoted as K 3 V 3 (PO 4 ) 4 /C has been achieved. K 3 V 3 (PO 4 ) 4 /C was subsequently employed as a novel positive electrode material for KIBs. Upon subjecting it to 100 cycles at a current density of 200 mA g −1 , the discharge specific capacity exhibited a remarkable value of 37 mAh g −1 , thus showcasing a capacity retention of 88%. Impressively, even after undergoing 300 cycles at a high current density of 400 mA g −1 , the capacity retention remained constant at 85%. The superior long-term cycling performance and high capacity retention observed in K 3 V 3 (PO 4 ) 4 /C can be attributed to the inherent stability of the polyanionic layered structure and the dual contributions derived from the carbon coating. Furthermore, the application of characterization techniques such as synchrotron X-ray absorption near-edge structure spectroscopy (XANES) revealed a V valence state of + 3 within the synthesized sample. By establishing a structural model for K 3 V 3 (PO 4 ) 4 /C and conducting first-principles calculations on its band structure and density of states, it was confirmed that the material facilitates electron transfer . An investigation into potassium ion migration and diffusion elucidated the involvement of tetrahedral site hopping (TSH). The successful synthesis of K 3 V 3 (PO 4 ) 4 /C material not only provides valuable insights but also serves as a reference for the development of KIBs cathode materials.
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ACS Catalysis
·
2023
·
IF 12.9
Shuai Xu,Qi Gao,Ziyan Hu,Yitong Lu,Yanlin Qin,Yuliang Li
The selective breaking of the Cβ–O bond has great potential for the conversion of lignin into high-value aromatic monomers. In the present work, we designed a CdS–SH/TiO2 heterojunction photocatalyst for the efficient selective breaking of the Cβ–O bond. The surface modification of CdS by –SH promoted close contact between the catalyst and lignin and further promoted the Fermi level matching with TiO2. A type-II heterojunction was constructed by CdS–SH and TiO2 nanosheets to enhance the light absorption range and further increase the separation of photogenerated electron–hole pairs, resulting in high catalytic activity. Finally, 85% phenol and 87% acetophenone yields were obtained under mild light irradiation using 2-phenoxy-1-phenylethanol as the model substrate. Several control experiments, along with DFT calculations, indicate that the reaction pathway is more likely to involve the oxidation of Cα–OH to form Cα═O initially, followed by the activation of Cβ–O, which is then reduced to further form aromatic monomers. This work achieves the efficient selectivity of lignin depolymerization and provides a reference for the design of heterojunction photocatalysts in the valorization of lignin.
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