BIOCHEMICAL ENGINEERING JOURNAL
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2020
·
IF 3.475
Yongxing Li,Pengqian Luan,Liya Zhou,Saiguang Xue,Yihang Liu,Yunting Liu,Yanjun Jiang,Jing Gao
The synthesis or decomposition of complex substances through the combination of metals and enzymes is desirable but still a huge challenge. A kind of yolk-shell structured Co/C@SiO 2 @Ni/C nanocomposites were prepared by the polyhedral ZIF-67@SiO 2 composite as a precursor through the extended stöber method and subsequent carbonization treatment. The SiO 2 as an intermediate protective layer stabilized the morphology and structure of the carbonized products. The metallic nickel nanoparticles were uniformly distributed on the surface of Co/C@SiO 2 @Ni/C for highly specific absorption of His-tagged organophosphohydrolase (OpdA) from cell lysates via affinity, and therefore an integrated nanocatalyst (INC) named OpdA@Co/C@SiO 2 @Ni/C was successfully prepared. The prepared INC was applied to achieve a one-pot chemoenzymatic cascade degradation of organophosphates (OPs) to p -aminophenol (PAP) within 30 min. In addition, the INC proved to be a simple and high-sensitivity nanocatalyst for the detection of methyl-parathion with a low limit of detection (0.30 μM). The INC exhibited improved pH stability, thermal stability, SDS resistance, and storage stability compared to that of free enzymes. When OpdA@Co/C@SiO 2 @Ni/C was reused for 7 cycles, the cascade degradation efficiency of methyl-parathion could retain more than 60 %. This study provides a strategy for constructing a multifunctional nanocatalyst, and further demonstrated its potential in biocatalysis, accurate detection of OPs and remediation of environmental pollution.
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Nanoscale
·
2016
·Vol. 8
·期 21
·10928-10937
·
IF 7.76
Hai-Bo Huang,Yue Yang,Li-Hua Chen,Yun Wang,Shao-Zhuan Huang,Jia-Wei Tao,Xiao-Ting Ma,Tawfique Hasan,Yu Li,Yan Xu,Bao-Lian Su
Engineering hierarchical structures of electrode materials is a powerful strategy for optimizing the electrochemical performance of an anode material for lithium-ion batteries (LIBs). Herein, we report the fabrication of hierarchical TiO2/C nanocomposite monoliths by mediated mineralization and carbonization using bacterial cellulose (BC) as a scaffolding template as well as a carbon source. TiO2/C has a robust scaffolding architecture, a mesopore–macropore network and TiO2–C heterostructure. TiO2/C-500, obtained by calcination at 500 °C in nitrogen, contains an anatase TiO2–C heterostructure with a specific surface area of 66.5 m2 g−1. When evaluated as an anode material at 0.5 C, TiO2/C-500 exhibits a high and reversible lithium storage capacity of 188 mA h g−1, an excellent initial capacity of 283 mA h g−1, a long cycle life with a 94% coulombic efficiency preserved after 200 cycles, and a very low charge transfer resistance. The superior electrochemical performance of TiO2/C-500 is attributed to the synergistic effect of high electrical conductivity, anatase TiO2–C heterostructure, mesopore–macropore network and robust scaffolding architecture. The current material strategy affords a general approach for the design of complex inorganic nanocomposites with structural stability, and tunable and interconnected hierarchical porosity that may lead to the next generation of electrochemical supercapacitors with high energy efficiency and superior power density.
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Materials
·
2016
·Vol. 9
·期 11
·913
·
IF 2.728
Guihua Cui,Zhengguo Gao,Nannan Qiu,Toshifumi Satoh,Toyoji Kakuchi,Qian Duan
Regioselective modification ofd-glucosamine (2-amino-2-deoxy-d-glucopyranose, GA) through C-1 and C-2 positions to synthesized thermo-responsive D-Glucosamine-poly(N-iso-propylacrylamide) (PNIPAM) via atom transfer radical polymerization (ATRP) was investigated for the first time. Two different schemes of the synthesis for GA derivatives (GA-PNIPAM (i) and (ii)) with well-defined structures using 3,4,6-tri-o-acetyl-2-deoxy-2-phthalimido-β-d-glucopyranose and 1,3,4,6-tetra-o-acetyl-2-amino-2-deoxy-β-d-glucopyranose intermediates were examined. The GA-PNIPAM (ii) had an amino at C-2 position, while there was a hydroxyl in GA-PNIPAM (i) at this position. Both the resulting oligomers (i) and (ii) had a narrow dispersity, and no significant cytotoxic response of copolymers (i) and (ii) was observed in the cell line over the concentration range from 0.1 μg/mL to 1000 μg/mL at any of the exposure times. In addition, it was discovered that GA-PNIPAM (i) and (ii) inhibited the proliferation of Human Hepatocellular Carcinoma Cells HepG2 as the concentration and the time changed, and the inhibitory activity of polymer (ii) was higher than that of he (i). The results suggest that the GA-PNIPAM polymers show excellent biocompatibility in vitro.Keywords:poly(N-isopropylacrylamide) (PNIPAM);d-glucosamine (GA);atom transfer radical polymerization (ATRP);lower critical solution temperature (LCST)
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ACS Applied Energy Materials
·
2024
·
IF 5.4
Yanting Ma,Yan Tang,Yajuan Xu,Suisui Su,Shuzhen Chen,Shizheng Zheng,Changyuan Hu,Xin Li,Kejie Dai,Rongbin Zhang
Metal oxides are promising alkaline battery electrodes with high theoretical capacity, but the low energy density and poor stability make them far away from actual application. Herein, single Bi-MOF derived ultrastable Bi2O3@C and BiOCl@C anodes are architected via a two-for-one manner. Specifically, optimal Bi2O3@C anode with hierarchical and porous structure delivers high specific capacity (278.3 mAh g–1 at 1 A g–1) owing to the exposed electrochemical active sites, fast charge transfer, and efficient ion diffusion. More importantly, ultrahigh stability (110%, 5000 cycles) is achieved due to the in situ morphological self-optimization and oxygen vacancy creation. Similarly, BiOCl@C anode also displays remarkable capacity and ultralong cycling stability (94%, 15000 cycles) due to the conductive and protective carbon layer, abundant reactive centers, and ion transport channels. Moreover, the in situ phase transition of BiOCl to Bi2O2CO3 also contributes to the outstanding stability. Our work provides rational guidance for architecting high capacitive and ultrastable anodes for aqueous rechargeable alkaline battery.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2024
·
IF 4.9
Gongheng Zhang,Abdullah Ali Mohammed Ahmed Al-Anzah,Fengxiang Yin,Jie Zhang,Guoru Li,Biaohua Chen,Qiuyue Gao,Xian Tong Yu,Yuqian Sun
The precursor ZIF-67/xC-T was prepared by solvothermal and pyrolysis methods. A series of ZIF-67/xC-T-yIL catalysts were then prepared by modifying the surface of the precursor with [BMIM][NTf 2 ] ionic liquid . The results showed that [BMIM][NTf 2 ] as sulfur and nitrogen sources, N, S co-doped carbon can improve the catalytic activity of ORR . Meanwhile, [BMIM][NTf 2 ] formed an oxygen-rich layer on the catalyst surface, which increased the contact between oxygen and the active sites, reduced the alkaline strength of the catalyst surface, and improved the desorption ability of the catalyst to the product. Therefore, the ZIF-67/xC-T-yIL catalyst exhibited better ORR activity in an alkaline electrolyte than the catalyst without [BMIM][NTf 2 ]. Among the ZIF-67/xC-T-yIL catalysts, ZIF-67/1.2 C-600–6IL demonstrated the best ORR catalytic activity, with a half-wave potential of 0.86 V and a limiting current density of 5.21 mA cm −2 in 0.1 mol L −1 KOH, which was comparable to that of commercial 20% wt% Pt/C.
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COLLOIDS AND SURFACES B-BIOINTERFACES
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2024
·
IF 5.4
Yuanyuan Wang,Weimin Guan,Yulin Yang,Huiling Lan,Yu Wang,Yun Wang,Juan Han,Lei Wang
Immobilization of enzymes in porous organic framework (POF) materials is popular strategy to stabilize enzymes. For such solid enzyme catalysis system, improving the catalytic efficiency is challenging due to the diffusion resistance from solid-liquid interface and inner pores. Here, UCST-pH dual responsive polymeric carrier (PEG- b -PAAm- b -P(GMA- co -AAc)) was synthesized to immobilize cytochrome c (Cyt c), which impart the reversibly insoluble-soluble property to the immobilized Cyt c. The PEG- b -PAAm- b -P(GMA- co -AAc) could serve as an insoluble-soluble matrix to fast and efficiently immobilize Cyt c via covalent attachment, achieving a remarkable 92 % loading efficiency within just 120 min. The obtained insoluble PEG- b -PAAm- b -P(GMA- co -AAc)-Cyt c micelles exhibited an improvement in thermal, pH stability and reusability. The completely soluble PEG- b -PAAm- b -P(GMA- co -AAc)-Cyt c conjugates accelerated substrate diffusion and then enhanced the catalytic efficiency. These excellent advantages led to low detection limit (1.99 μM), lower than the presently reported biosensors based on enzyme mimics in the colorimetric detection of phenol. This UCST-pH dual responsive window presents a new platform to efficiently control the immobilization and release of enzymes, which will achieve excellent stability and catalytic efficiency.
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Science China-Chemistry
·
2025
·
IF 9.7
Kang Kai,Wang Qiuxiang,Huang Hongpu,Zhuang Xinxin,Cai Junlin,Wang Tao,Wang Xue,Xie Zhaoxiong,Xie Shuifen
Despite utilization of state-of-the-art Cu-based catalysts, achieving high selectivity and stability in multicarbon (C 2+ ) compounds production through electrocatalytic CO 2 reduction reaction (CO 2 RR) remains a critical and challenging objective. Here we employ lattice chlorine-doped Cu 2 O nanocubes (Cl d -Cu 2 O NCs) with well-defined {100} facets as a model catalyst to demonstrate that halogen doping can serve as a versatile and effective strategy for modulating surface charge distribution, thereby enhancing asymmetric C–C coupling toward high-selectivity C 2+ products in CO 2 RR. Compared to Cl-free Cu 2 O NCs, Cl d -Cu 2 O NCs exhibit a greatly enhanced C 2+ Faraday efficiency, i.e., ∼85% at −1.1 V (versus the reversible hydrogen electrode). Additionally, the Cl d -Cu 2 O NCs demonstrate significantly enhanced long-term durability, attributed to better preservation of the cubic morphology and more stable Cu δ + states. In-situ electrochemical studies reveal that Cl d -Cu 2 O NCs facilitate the formation of the key asymmetric *COH and *OCCOH intermediates, ultimately leading to higher C 2+ products. Density functional theory (DFT) calculations confirm that the introduced Cl-dopants disrupt the charge balance of the Cu 2 O(100) surface, enriching the Cl-adjacent Cu atoms with more electrons compared to those near O atoms. This unbalanced charge distribution significantly reduces the free energy of the rate-determining step for asymmetric C–C coupling from the *CO to *OCCOH on Cl-doped Cu 2 O (100) surface, requiring only 1.04 eV, in contrast to 1.50 eV on pristine Cu 2 O(100) surface. This study provides valuable insights into the surface charge modulation of Cu 2 O catalysts via halogen doping for enhancing asymmetric C–C coupling and C 2+ production in CO 2 RR.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Xuan Qi,Jun-Hao Wang,Jiang Shao,Hao Dong,Chen Li,Ya-Wen Zhang
Efficient production of multi-carbon (C₂ ⁺ ) products via CO 2 electroreduction reaction (eCO 2 RR) requires precise modulation of water activation, but still less investigated. In this work, we synthesized series of rare earth hydroxide-modified copper-based catalysts (RE(OH) 3 /CuO) to enhance water activation at the heterogeneous interfaces. Electrochemical evaluation showed significantly increased Faradaic efficiency for C₂ ⁺ products (up to 77.2 % at 500 mA cm −2 ) for the Sm(OH) 3 /CuO catalyst, alongside suppressed hydrogen evolution reaction (HER). This is caused by the facilitated hydrogenation of critical *CO intermediates via hydrogen spillover from the abundant Sm(OH) 3 /CuO interfaces in efficiently dissociating water molecules, promoting asymmetric C–C coupling on the Cu surfaces derived from CuO during eCO 2 RR. Experimental findings combined with DFT calculations indicated the critical role of the asymmetric *CO–*CHO coupling pathway on copper surfaces. This strategy demonstrates that rational design of interface water engineering and activation for a copper-based heterogeneous catalyst effectively promotes multi-carbon product formation in eCO 2 RR.
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ACS Catalysis
·
2025
·
IF 13.1
Rui Zhai,Zhenyu Wang,Chang Huang,Chao Zeng,Mengyue Gu,Tianqi Wang,Fanqi Bu,Shaobin Wang,Jinying Zhang
Phosphorus has various crystallographic structures and variable phosphorus-derived structures, which have attracted much attention due to its unique properties. One-dimensional phosphorus structures with atomic substitution in the phosphorus lattice are extremely favored due to their high specific surface area and stable single-atom dispersion. The precise crystal structures and single atomic substitution positions are crucial factors to understand the mechanism of single-atom effects but remain a big challenge. Herein, single crystals composed of 1D zigzag linear phosphorus selenium chains (ZLP-Se) have been produced and characterized by SC-XRD to be P18.56Se1.44 with a space group of Pnma (CSD-2348033). The exact Se substitution positions were further ascertained by calculations of the whole thermodynamic stability phase diagram to have three types of substitution patterns (Se1/P1 mixed occupied positions with intervals of 3Se+2P, 1Se+4P, and 1Se+1P+1Se+2P). The selenium-rich crystal plane (-10-1) has been demonstrated to significantly enhance CO2 adsorption and C−C coupling to obtain ethylene (C2H4). A high photocatalytic CO2 reduction performance (18.0 μmol g−1 h−1, 97.0% electron selectivity for C2H4) has been achieved by the ZLP-Se with the Ag cocatalyst. The adsorption of CO2* and CO* was found to be much stronger on the Se-rich surface of ZLP-Se. The CO* intermediates were found to be energetically favored for protonation and subsequent asymmetrical C−C coupling to produce C2H4, with COCHO* intermediates detected by in situ DRIFTS. The electron was also demonstrated by in situ XPS to transfer from Se and Ag to P under Xe lamp irradiation, confirming the electronic localization effect of ZLP-Se to yield C2H4.
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INTERNATIONAL JOURNAL OF POLYMER ANALYSIS AND CHARACTERIZATION
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2025
·
IF 1.6
Junxia Chai,Hongbo Mo,Chuan Wang,Fengjie He,Jufen Huang,Li Ran,Weigang Fan,Yuepeng Fan,Fan Lu
This study developed Fe3O4@SiO2–C = C-based magnetic molecularly imprinted polymers for selective ibuprofen removal and detection. The optimized synthesis using an ibuprofen (IBP)/(3-aminopropyl)triethoxysilane (APTES)/tetraethyl orthosilicate (TEOS) molar ratio of 1:6:18 achieved a high adsorption capacity of 68.18 mg·g−1 and an imprinting factor of 2.17. The adsorption process followed pseudo-second-order kinetics and the Freundlich isotherm model, indicating multilayer binding behavior. The material demonstrated excellent reusability with only 2.8% capacity loss after five cycles and good reproducibility with a relative standard deviation of 4.48%. In magnetic solid-phase extraction applications, the recovery rate reached 81.61% to 96.40% for real water samples with a detection limit of 0.09 μg·mL−1. The polymers showed selective recognition of ibuprofen over structural analogs due to synergistic π-π interactions and hydrogen bonding, thus offering an efficient strategy for remediating pharmaceutical pollutants in water.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Huaqing Chen,Yuyan Wang,Shujia Zhang,Yuting He,Linrui Hou,Changzhou Yuan
Rechargeable Zn-ion batteries (ZIBs) have attracted much attention due to their high energy density, high safety, and low cost. Nevertheless, the practical implementation of ZIBs has been dreadfully hindered by the lack of stable high-capacity cathode candidate and serious dendritic growth in Zn anode. Superior device-level performance can only be achieved by simultaneously addressing the fatal shortcomings of both electrodes. Herein, we explore a two-pronged approach to achieving high-capacity, long-life stable ZIBs via synergistic design in both anodes and cathodes. Specifically, hierarchical accordion-like ZnV 2 O 4 @C (A-ZVO@C) framework derived from multi-layered V 2 CT x is fabricated and endowed with high electronic/ionic conductivities and structural/chemical stability, exhibiting striking high-rate capacities/stability when utilized as a cathode. Meanwhile, a dendrite-free Zn with an artificial protective layer of zincophilic ZnO/C hollow spheres affords outstanding Zn plating-stripping stability with a prolonged lifespan, which reduces local current density, homogenizes Zn 2+ ion diffusion/deposition, and suppresses volume changes during long-term plating/stripping. As a result, the assembled full ZIBs deliver a high-rate capacity of 232.2 mAh g −1 at 8 A g −1 , and superb stability with capacity degradation of 7.8 % over 3000 consecutive cycles at 15.0 A g −1 . More meaningfully, the contribution here provides an essential guidance for rationally designing next-generation ZIBs.
研究领域:
能量存储
·
材料科学
·
电化学
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WATER RESEARCH
·
2020
·
IF 9.13
Da Kang,Yiyu Li,Dongdong Xu,Wenji Li,Wei Li,Aqiang Ding,Ru Wang,Ping Zheng
The red color is the most striking character of anaerobic ammonium-oxidizing bacteria (AnAOB) which has been used to estimate the anammox activity roughly. However, the quantitative relationship between the color and activity of anammox sludge still remains unknown. In this study, the chromaticity, activity and their correlation were systematically investigated at different steady-state nitrogen loading rates. The chromaticity of anammox sludge was digitalized by the CIE L*a*b* color space. The results revealed that the average chroma value was found to be significantly correlated with specific anammox activity ( r = 0.940, p < 0.01) and the cluster centers of chromaticity coordinates (a*, b*) of anammox sludge were established to define the typical working states of anammox system. The visible spectra of anammox sludge were proved to originate from the cytochrome c. The correlation between chroma and heme c concentration of anammox sludge was consistent with the fully-reduced cytochrome c and the chroma was determined by both content and redox ratio of cytochrome c. The chromaticity of anammox sludge was able to be linked with the anammox activity via reduced cytochrome c content. The gene abundance of cytochrome c synthetase linked the chromaticity with AnAOB quantity via total cytochrome c content, while the enzyme activity of octaheme hydrazine dehydrogenase linked the chromaticity with AnAOB activity via reduced cytochrome c ratio. Moreover, the redundancy analysis proved that heme c, as the key component of cytochrome c, was the most important explanatory variable accounting for the maximum 69.6% of the total variation of the anammox community, which correlated positively with the relative abundance of dominant AnAOB ( Candidatus Kuenenia). This work aimed at demonstrating the chromaticity of anammox sludge could be developed as an alternative intuitive anammox activity indicator which will promote the monitoring and optimization of anammox process.
研究领域:
环境工程
·
微生物学
·
生物技术
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高影响因子
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