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Bionically mineralized ZIF-67-derived adjustable mesoporous FeCoO_x/C efficiently immobilize horseradish peroxidase for chloridazon degradation via Fenton and enzyme synergistic catalysis

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Chemical engineering Journal 2025年 517卷

作者： Jing, Lingyun Hu, Yeqiang Wang, Tong Hao, Pengbo Sun, Zhili Zhao, Xia Yin, Fei Zhang, Dongnian Yang, Hui Zheng, Yinqin Li, Xinyong Liu, Shasha Zhang, Zeqiang Zhu, Hao College of Petroleum and Chemical Engineering Lanzhou University of Technology Lanzhou 730050 China Key Laboratory of Western China's Environmental Systems (Ministry of Education) and Lanzhou University-Jinchuan Group Chemical Co. Ltd. Chemical Environmental Protection Industry Joint Laboratory College of Earth and Environmental Sciences Lanzhou University Lanzhou 730000 China Ministry of Education Key Laboratory for Non-equilibrium Synthesis and Modulation of Condensed Matter Shaanxi Province Key Laboratory of Advanced Functional Materials and Mesoscopic Physics School of Physics Xi'an Jiaotong University Xi'an 710049 China School of Ecology and Environment Ziyang College of Environmental Science and Technology Ziyang 641300 China

Immobilized enzyme technology, as a green catalytic method, is often limited by the immobilization performance, stability, and inherent activity. Herein, an immobilization strategy based on ZIF-67-derived FeCoO_x/C (mFCZ) was proposed for the degradation of chloridazon (CLZ). By embedding bovine serum albumin (BSA) during the preparation process of ZIF-67, mesoporous FeCoO_x/C materials with sizes matching (pore size of 13.787 nm) horseradish peroxidase (HRP) were prepared after carbonization. The enzyme loading capacity of mFCZ/HRP could reach 89.6 % (199.7 mg/g). Its specific surface area and pore size were 28.975 m²/g and 5.89 nm, respectively. The mFCZ possessed dispersed active metal oxide sites, FeCoO_x. The material significantly enhanced the stability and activity of the enzyme (440.97 U/g). In addition, the mFCZ/HRP exhibited excellent electrical conductivity. The mFCZ/HRP/H₂O₂ synergistic system prominently facilitated the degradation of CLZ. The synergistic system reached 95.37 % within 90 min, with a rate constant of 0.034 min⁻¹, which was 19 times and 2.5 times higher than the Free HRP/H₂O₂ system (0.002 min⁻¹) and the mFCZ/H₂O₂ system (0.014 min⁻¹), respectively. This enzyme-Fenton synergistic mechanism was proposed that the electrons generated by HRP catalysis promoted the valence conversion of Co and Fe, thereby accelerating the formation and reaction rate of ·OH to degradate CLZ. This work provides new insights into the enzyme-Fenton synergistic catalytic degradation of pollutants. © 2025 Elsevier B.V.

关键词： Chloridazon (CLZ) Fenton-like technology Immobilized enzyme Pore-confinement Synergistic catalysis

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Difference in Cd2+ Flux Around the Root Tips of Different Soybean (Glycine Max L.) Cultivars and Physiological Response Under Mild Cadmium Stress

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SSRN 2022年

作者： Wang, Siqi Dai, Huiping Skuza, Lidia Chen, Yanqiu Wei, Shuhe Key Laboratory of Wastewater Treatment Technology of Liaoning Province Academy of Environmental & Chemical Engineering Shenyang Ligong University Liaoning Shenyang110159 China College of Biological Science & Engineering Shaanxi Province Key Laboratory of Bio-resources Qinling-Bashan Mountains Bioresources Comprehensive Development C.I.C State Key Laboratory of Biological Resources and Ecological Environment Jointly Built by Qinba Province and Ministry Shaanxi University of Technology Hanzhong723001 China Key Laboratory of Pollution Ecology and Environment Engineering Institute of Applied Ecology Chinese Academy of Sciences Shenyang110016 China Institute of Biology Centre for Molecular Biology and Biotechnology University of Szczecin Szczecin71-415 Poland Crop Institute Liaoning Academy of Agricultural Science Liaoning Shenyang110161 China

The purpose of the study was to compare differences in Cd2+ flux in the vicinity of root tips of various soybean cultivars under mild Cd stress conditions using non-invasiv... 详细信息

The purpose of the study was to compare differences in Cd2+ flux in the vicinity of root tips of various soybean cultivars under mild Cd stress conditions using non-invasive micro-test technology (NMT). The results indicated that Cd2+ influx to the root tips under mild Cd treatment was higher compared to controls. Cd2+ influx showed an obvious spatial distribution, with the highest Cd2+ influx measured 300 μm from the root tips, and a gradually decrease above and below this site. The cultivar Liaodou32 had a lower Cd uptake (3.40 pmol cm-2 s-1), while Liaodou23 had a relatively higher Cd uptake (66.37 pmol cm-2 s-1). Cluster analysis showed that the order of the average Cd2+ influx of the cultivars at a distance of 300 μm from the root tips was as follows: high-uptake cultivars (61.80 pmol cm-2 s-1)＞medium-high-uptake cultivars (33.92 pmol cm-2 s-1)＞medium-low-uptake cultivars (19.78 pmol cm2 s-1)＞low-uptake cultivars (4.84 pmol cm-2 s-1). We also analyzed physiological responses of different soybean cultivars to mild Cd stress. The results indicated that mild Cd stress could inhibit soluble protein production and root vigor among individual soybean cultivars. Moreover, stress increased SOD, CAT and POD activities and MDA content in root tissues. It should be noted that the physio-biochemical indicators of low-uptake cultivars did not change significantly after exposure to mild Cd stress compared to controls. Pearson’s correlation analyses showed that all physio-biochemical indicators were significantly positively associated with influx, except of root SP and biomass. PCA analysis demonstrated that root vigor was a dominant factor causing the differences in Cd tolerance among different soybean seedling cultivars. Soybean seedling cultivars with parallel Cd uptake had similar physio-biochemical characteristics under Cd stress. © 2022, The Authors. All rights reserved.

关键词： Amino acids

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Dual Functional Mesoporous Silica Colloidal Electrolyte for Lithium-Oxygen Batteries

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SSRN 2022年

作者： Mu, Hailiang Zhuge, Xiangqun Ren, Guogang Luo, Kun Ding, Zhengping Ren, Yurong Luo, Zhihong Bayati, Maryam Xu, Ben Bin Liu, Xiaoteng Changzhou Key Laboratory of Intelligent Manufacturing and Advanced Technology for Power Battery School of Materials Science ＆ Engineering Changzhou University Changzhou213164 China Department of Engineering and Technology School of Physics Engineering and Computer Science University of Hertfordshire Hertfordshire HatfieldAL10 9AB United Kingdom Guangxi Key Laboratory of Optical and Electronic Materials and Devices Guilin University of Technology Guilin541004 China Department of Mechanical and Construction Engineering Faculty of Engineering and Environment Northumbria University Newcastle upon TyneNE1 8ST United Kingdom

Dual functional mesoporous silica (mSiO2) colloidal electrolytes are designed for lithium-oxygen batteries (LOBs) for the purpose of protecting lithium anode and accelerating cathode reaction kinetics. It suppresses the side reactions of Li stripping/plating and enhances the cycling life performance of the LOB by relieving the attack of superoxide intermediates. The co-deposition of mesoporous mSiO2 and Li2O2 also effectively accelerated the decomposition of the discharge product by promoting the mass transfer at the cathode. Testing results show that the battery life of LOB using mSiO2 with a concentration of 80 mg L-1 in the colloidal electrolyte has been extended from 55 to 328 cycles compared with the one using conventional LiClO4/DMSO electrolyte. The rate performance and full-discharge capacity are also significantly enhanced. We discovered that the as-synthesized mSiO2 has a special well-ordered hexagonal mesoporous structure, with a high specific surface area of 1016.30 m2 g-1, which can form a stable colloid after mixing with 1.0 M LiClO4/DMSO. This is a meaningful investigation of suppressing side reactions using non-aqueous electrolytes, and the design principle also impacts research on other types of lithium metal batteries. © 2022, The Authors. All rights reserved.

关键词： Electrolytes

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Eg Obital Occupancy-Dependent Intrinsic Catalytic Activity of Zn-Co-Mn Spinel Oxides for Peroxymonosulfate Activation

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SSRN 2022年

作者： Li, Wenqian Cheng, Haijun Zhang, Lijuan Wang, Xiaopeng Qian, Kun Zhang, Bin Ma, Jun He, Xu State Key Laboratory of Urban Water Resource and Environment Harbin Institute of Technology Harbin150090 China Key Laboratory of Interfacial Physics and Technology Chinese Academy of Sciences Shanghai 201800 China Shanghai Synchrotron Radiation Facility Shanghai Institute of Applied Physics Chinese Academy of Sciences Shanghai 201204 China National Key Laboratory for Precision Hot Processing of Metals Harbin Institute of Technology Harbin150001 China State Key Laboratory of Pollution Control and Resources Reuse College of Environmental Science and Engineering Tongji University Shanghai 200092 China

Transition metal (TM)-based spinel oxides have demonstrated excellent efficacy in Fenton-like reactions, but the existing model cannot fully explain the origin of catalytic activity. Here, we first discover a critical role of eg occupancy in governing the intrinsic activity of ZnCoxMn2-xO4 spinel oxides (x=0-2.0) for peroxymonosulfate (PMS) activation and pollutant degradation. The introduction of Co into ZnMn2O4 network lowers magnetic momentum, eg occupancy, and favors the overlap between TM eg and O 2p orbitals. ZnCo2O4 with optimal eg occupancy, favorable PMS binding strength, interaction capability, and radical desorption exhibits the best catalytic activity. Cyclic voltammetry (CV) and Density functional theory (DFT) corroborate that ZnMn2O4 (eg=0.97) exhibits inert activity due to weak affinity towards PMS. The eg occupancy from 0.43 in ZnCo2O4 to 0.77 in ZnCoMnO4 is found to weaken PMS binding. These useful insights may inspire the reasonable development of catalysts, assist the prediction and enhancement of catalytic activity. © 2022, The Authors. All rights reserved.

关键词： Catalyst activity

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Cleaning Mechanism of Gypsum Scaling in Hydrophobic Porous Membranes

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SSRN 2022年

作者： Xie, Songchen Wong, Ngie Hing Sunarso, Jaka Guo, Qiang Hou, Chunguang Pang, Zhiguang Peng, Yuelian Beijing Key Laboratory for Green Catalysis and Separation Faculty of Environment and Life Beijing University of Technology Beijing100124 China Research Centre for Sustainable Technologies Faculty of Engineering Computing and Science Swinburne University of Technology Jalan Simpang Tiga Sarawak Kuching93350 Malaysia State Key Laboratory of Water Resource Protection and Utilization in Coal Mining Beijing102208 China

Mineral scaling is one of the major challenges for membrane distillation in concentrating high salinity *** work first investigated the characteristic of CaSO4 scaling, then explored different cleaning reagents to evaluate their efficiencies and mechanisms. By analyzing the SEM and EDX mapping images, the CaSO4 scaling process could be divided into surface and pore scaling stages. Three cleaning solutions, i.e., commercial detergent (20%), EDTA-4Na (0.05 M), and MgCl2 (0.8 M), were chosen for their high CaSO4 solubility (0.7 g CaSO4 per 100 g H2O).At the surface scaling stage, three cleaning solutions exhibited excellent removal of CaSO4 scaling with approximately similar 96% cleaning ***, at the pore scaling stage, only the commercial detergent showed high efficiency (89%).Such high cleaning efficiency was mainly attributed to the detergent's high total dissolved solids (salinity), low pH, and high diffusion rate (5.19 µm cm-1 min-1 ) across the ***, periodic cleaning at the surface scaling stage with the commercial detergent followed by drying throughout a 43.5 h continuous concentration test on an actual RO brine could restore the PTFE membrane performance completely, giving 90% of the total water *** work provides a new insights into the cleaning mechanism for gypsum scaling in hydrophobic porous membrane. © 2022, The Authors. All rights reserved.

关键词： Calcium sulfate

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Bisthiourea Immobilized Uio-66-Nh2 Supported Fe2o3 Nanoparticles to Accelerate Dual Centers Fenton-Like Reaction

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SSRN 2022年

作者： Huang, Xu Fan, Xiaohu Li, Aimin Tian, Yechao Li, Dawei State Key Laboratory of Pollution Control and Resource Reuse School of Environment Nanjing University Nanjing210023 China School of Water Conservancy and Civil Engineering Northeast Agricultural University Heilongjiang Harbin150030 China School of Environmental Science and Engineering Nanjing University of Information Science & Technology Nanjing210044 China

In this paper, an efficient catalyst UiO-66-BTU/Fe2O3 was synthesized by using bisthiourea modified Zirconium-based Metal Organic Framework (Zr-MOF). The UiO-66-BTU/Fe2O3 system features outstanding Fenton-like activity that is 20.38 times and 11.52 times larger than Fe2O3 and conventional UiO-66-NH2/Fe2O3 system. It also exhibits good stability, broad pH range and recycle ability. Through comprehensive mechanistic investigations, we have ascribed the excellent catalytic performance of the UiO-66-BTU/Fe2O3 system to 1O2 and HO• as the reactive intermediates, cause Zr centers can make complexation with Fe to form dual centers. Meanwhile, the C=S on the bisthiourea can form Fe-S-C bonds with Fe2O3, reducing the redox potential of Fe(III)/Fe(II) and influencing the decomposing of H2O2, which indirectly regulate the interaction between Fe and Zr to accelerate electron transfer during the reaction. This work exhibits the design and understanding of the iron oxides incorporated in modified MOFs with excellent Fenton-like catalytic performance to remove phenoxy acid herbicides. © 2022, The Authors. All rights reserved.

关键词： Redox reactions

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DNAzyme-Powered AuNRs-DNA Walker for Visual Detection of Escherichia Coli

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SSRN 2023年

作者： Li, Zongqiang Li, Jingjing Wang, Xu Li, Qianru Zhu, Jingru Yao, Yuying Guo, Zhiqiang Wang, Yu Liu, Su Huang, Jiadong School of Biological Sciences and Technology University of Jinan Jinan250022 China Shandong Institute of Metrology and Science Jinan250014 China School of Water Conservancy and Environment University of Jinan Jinan250022 China Key Laboratory of Chemical Sensing and Analysis in Universities of Shandong School of Chemistry and Chemical Engineering University of Jinan Jinan250022 China

Escherichia coli (E. coli) is a common Gram-negative bacterium that is widely distributed in nature and is susceptible to natural and random genetic factors. It is a pathogenic factor for many diseases. Sensitive and specific detection of E. coli is an important means to ensure food safety and prevent foodborne disease outbreaks. Ultrasensitive and specific detection of E. coli is still an urgent problem to be solved. An intuitive and convenient colorimetric assay method with high sensitivity was proposed here for E. coli based on a DNAzyme-powered AuNRs-DNA walker. The strategy, dependent on the targeted activation of Mg2+-DNAzyme, starts an efficient DNA walking machine, induces the formation of countless peroxidase-mimicking enzymes, and produces color change via chromogenic reaction for visual detection of E. coli. The strategy has the following features. Firstly, this is the first time that an AuNRs-based DNA walker is integrated with a colorimetric assay of E. coli. Through the combination of DNAzyme-powered AuNRs-DNA walker and visual detection via the peroxidase-mimicking enzyme, the detection sensitivity is significantly improved compared to the previous colorimetric-based methods, which provides a paradigm for the development of highly sensitive colorimetric assay methods. Secondly, activity-controlled nano-DNAzyme is constructed by target-triggered formation of G-quadruplex DNAzyme to achieve low background and high signal-to-noise detection. In addition, this strategy has the advantages of simple operation, short analysis time, low cost, and easy on-site detection. Therefore, the proposed strategy has the potential to be applied to the detection of E. coli and related food safety analysis and clinical diagnosis. © 2023, The Authors. All rights reserved.

关键词： DNA

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A Study of Co-Pyrolysis of Sewage Sludge and Rice Husk for Syngas Production Based on a Cyclic Catalytic Integrated Process System

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SSRN 2023年

作者： Pan, Xuwei Wu, Yan Li, Tingzhen Lan, Guoxin Shen, Jia Yu, Yue Xue, Ping Chen, Dan Wang, Maoqing Fu, Chuan Key Laboratory of Water Environment Evolution and Pollution Control in Three Gorges Reservoir Chongqing Three Gorges University Wan Zhou404100 China College of Environmental Science and Engineering Beijing Forestry University Beijing100083 China Chongqing GreenKarbon Environmental Protection Technology Co. Ltd. Chongqing400050 China

To promote higher-quality syngas production from biomass co-pyrolysis, this study prepared syngas through the secondary cracking of tar in cyclic catalytic pyrolysis steam based on a cyclic catalytic integrated pyrolysis (CCIP) system, the CCIP system process parameters were synergistically optimized based on the syngas yield and lower heating value (LHV) as indicators. The results showed that the mixing ratio and cycle rate was crucial to driving syngas generation, while the cycle rate was a key factor for tar reduction. The catalyst dosage mainly changed the syngas composition and promoted the generation of hydrogen-rich syngas. Optimization of the CCIP system reduced the liquid phase product yield by 6 wt.% and increased the gas product yield by 27 wt.% compared to the normal pyrolysis system based on sewage sludge (SS) pyrolysis, where the yields of H2, CH4, CO, and CO2 were increased by 131.51, 87.80, 223.57, and 210.45 vol%, respectively. The syngas LHV increased from 7.99 MJ/Nm3 to 11.31 MJ/Nm3 by 41.55 % through synergistic optimization. The co-pyrolysis of SS and rice husk and the development of pyrolysis tar reforming through pyrolysis steam circulation effectively improved the yield and LHV of syngas and achieved high-quality syngas recovery based on the CCIP system. © 2023, The Authors. All rights reserved.

关键词： Sewage sludge

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Characterization and Infrared Stealthy Properties of Two Schiff-base Compounds Derived from 1-Amino-2-hydroxypropane and Their Complexes

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Chinese Journal of Structural Chemistry 2020年第2期39卷 279-286,185页

作者： WEN Hui-Liang LAI Bo-Wen PENG Hua-Long XIONG Zhi-Qiang LIU Chong-Bo State Key Laboratory of Food Science and Technology Nanchang UniversityNanchang 330047China Chemicals Analysis Department Nanchang Institute for Food and Drug ControlNanchang 330038China School of Environment and Chemical Engineering Nanchang Hangkong UniversityNanchang 330063China

Single crystals of two Schiff base compounds 1 and 2 derived from 1-amino-2-hydroxypropane were obtained via condensation reaction of an amine and a reactive carbonyl group. The compounds were characterized by elemental analysis, IR and single-crystal X-ray diffraction. Compound 1(C(10)H(13)NO2) crystallizes in the monoclinic system, space group P21 with a = 4.487(9), b = 10.913(2), c = 9.886(19) ?, β = 97.823(3)o, V = 479.59(16) ?~3, Z = 2, Mr = 179.21, Dc = 1.241 g/cm^3, F(000) = 192, GOOF = 1.005, μ = 0.087 mm^(-1), the final R = 0.0328 and wR = 0.0738 for 1721 observed reflections with I > 2σ(I). Compound 2(C(14)H(20)N2O2) crystallizes in orthorhombic system, space group Pbca with a = 6.295(2), b = 7.290(3), c = 30.519(11) ?, V = 1400.5(9)?~3, Z = 8, Mr = 248.32, Dc = 1.178 g/cm^3, F(000) = 536, GOOF = 1.125, μ = 0.079 mm^(-1), the final R = 0.0871 and w R = 0.1748 for 1307 observed reflections with I > 2σ(I). Compound 1 exhibits a 3D supramolecular structure and compound 2 show a 3D supramolecular structure under hydrogen bonding interactions. Furthermore, the infrared stealthy performance of two Schiff base compounds and their Fe(Ⅲ) complexes were studied. The results show that their Fe(Ⅲ) complexes show lower infrared emissivity than corresponding Schiff base compounds, and the lowest infrared emissivity reaches to 0.657.

关键词： two Schiff base compounds 1-amino-2-hydroxypropane crystal structure Fe(Ⅲ)complexes infrared stealth

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Unveiling the Synergistic Catalysis Essence of Trimetallic Fe-Co-Ni Phosphides for Lithium–Sulfur Chemistry

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SSRN 2022年

作者： Yang, Qin Wei, Xijun Cao, Xuan Chen, Le Song, Lixian Kong, Long Sun, Wei Xie, Kefeng Song, Yingze State Key Laboratory of Environment-Friendly Energy Materials School of Materials and Science Engineering Southwest University of Science and Technology Sichuan Mianyang621010 China Frontiers Science Center for Flexible Electronics Xi'an Institute of Flexible Electronics Northwestern Polytechnical University Shaanxi Xi'An710129 China State Key Laboratory for Modification of Chemical Fibers and Polymer Materials College of Materials Science and Engineering Donghua Univeristy Shanghai201620 China School of Chemistry and Chemical Engineering Lanzhou Jiaotong University Gansu Lanzhou730070 China

Lithium–sulfur batteries (LSBs) have emerged as prospective candidates for energy storage systems due to their high energy density and low cost of sulfur. However, the fast capacity degradation stemming from the fatal lithium polysulfide (LiPS) shuttle and sluggish redox reaction kinetic acts as the bottleneck for the real implementation of LSBs. Herein, we propose a well-designed nanosphere functionalized with trimetallic Fe-Co-Ni phosphides (FCNP) to host sulfur and promote the sulfur redox reactions. The well-dispersed trimetallic phosphides can not only enhance polarity and electron conductivity but also supply sufficient conversion sites and short sulfur evolution pathway. Therefore, the elaborated trimetallic phosphides on carbon nanosphere effectively inhibits LiPSs escaping from the cathode to anode. Further, the systematic electrochemical measurements and synchrotron X-ray three-dimensional nano-computed tomography (X-ray 3D nano-CT) results provide clear evidence that FCNP as a bidirectional electrocatalyst smoothly accelerates the generation and decomposition of Li2S. Accordingly, the S/FCNP cathode exhibits a remarkable discharge capacity of 1172.3 mA h g–1 at 0.2 C in coin cell, 1164.0 mA h g–1 at 0.1 C in pouch cell and the favorable cycling performance. © 2022, The Authors. All rights reserved.

关键词： Redox reactions

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