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An orthogonal dual-regulation strategy for sensitive biosensing applications

National science Review 2022年第9期9卷 246-259页

作者： Xian Yang Jinhua Wang Zhongfeng Gao Weiqi Zhang Hai Zhu Yongjun Song Quan Wang Mingjie Liu Lei Jiang Yu Huang Fan Xia State Key Laboratory of Biogeology and Environmental Geology Engineering Research Center of Nano-Geomaterials of Ministry of EducationFaculty of Material Science and ChemistryChina University of Geosciences State Grid Integrated Energy Service Group CO.LTD. State Key Laboratory of Proteomics Beijing Proteome Research Center National Center for Protein Sciences(Beijing)Beijing Institute of Lifeomics Shandong Provincial Key Laboratory of Detection Technology for Tumor Markers College of Chemistry and Chemical Engineering Linyi University Key Laboratory of Bio-Inspired Smart Interfacial Science and Technology of the Ministry of Education School of Chemistry and EnvironmentBeihang University Zhejiang Institute China University of Geosciences

Biosensing systems based on controllable motion behaviors of droplets have attracted extensive attention,but still face challenges of insufficient sensitivity and uncontrollable dynamic range due to imprecise manipulation of droplet motion on the ***,we report an orthogonal dual-regulation strategy for precise motion control of droplets and we demonstrate its utility as a sensitive sensing system with controllable dynamic ranges of sensing for adenosine triphosphate,miRNA,thrombin and kanamycin,as well as discrimination of five kinds of D *** endowed a DNA-contained bio-droplet sliding on a lubricant-infused structural surface with micro-grooves to separately adjust the resistance from liquid phase and solid *** resistance from liquid phase mainly depended on hydrophobic interaction between DNA and lubricant,which can be finely tuned by different DNA's average chain ***,the resistance from solid surface was determined by the energy barrier from the periodic micro-grooves,which can be adjusted by varying the droplet's sliding direction on the *** hydrophobic interaction is conformed to be orthogonal to the micro-grooves' anisotropic resistance by three different *** orthogonal dual-regulation strategy thus demonstrated its ability to precisely control bio-droplets' motion behaviors and sensitive detection with adjustable dynamic ranges for various *** dual-regulation strategy will provide significant insights for super-wettable biosensors,visual inspection and beyond.

关键词： motion behavior sensitive detection dynamic range hydrophobic interaction anisotropic resistance

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Waste to Wealth: H2s-Free Fabrication of Fe-Zns/Nc by Industrial Lignin Self S-Doping for Efficient Lignin Aerobic Oxidation

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SSRN 2023年

作者： Guo, Haiwei Chen, Zhao Yin, Qiqi Sun, Tian Liu, Yuxuan Ren, Gengbo Li, Changzhi School of Energy and Environmental Engineering Hebei University of Technology Tianjin300401 China Shaanxi Key Laboratory of Low Metamorphic Coal Clean Utilization School of Chemistry and Chemical Engineering Yulin University Yulin719000 China CAS Key Laboratory of Science and Technology on Applied Catalysis Dalian Institute of Chemical Physics Chinese Academy of Sciences Dalian116023 China

Industrial lignin mostly contains sulfur, which poisons metal catalysts easily. Metal sulfides with good S-resistance could be used as efficient catalysts for lignin oxidation, while metal sulfides preparation involved corrosive H2S. Here in, we proposed H2S-free fabrication of bimetallic Fe-ZnS/NC by industrial lignin self S-doping. The Fe-ZnS/NC exhibited efficient oxidation activity (> 99% conversion) and good S-resistance for β-O-4 and industrial lignin oxidation. Density functional theory revealed the synergistic effect of FeS and ZnS in lignin oxidation, where FeS tended to activate O2 into superoxide radical (O2-•) and ZnS contributed to the polarization of β-O-4. The dual sites greatly reduced the migration distance of O2-• to the polarized β-O-4, facilitating the C-O/C-C cleavage. Hence, Fe-ZnS/NC selectively converted lignin into carbonyl-containing aromatics with up to 92% selectivity under alkaline-free condition. This work developed a novel strategy using lignin-derived metal sulfide without external sulfur source for efficient lignin degradation. © 2023, The Authors. All rights reserved.

关键词： Lignin

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Chromatic Acclimating Synechococcus Dominate in Mesoscale Eddies

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Journal of Geophysical Research: Oceans 2024年第7期129卷

作者： Zhang, Xiaodong Li, Yingdong Xu, Zhimeng Chen, Jiawei Cheung, Shunyan Jing, Hongmei Xu, Jie Liu, Hongbin Department of Ocean Science The Hong Kong University of Science and Technology Institute of Marine Biology National Taiwan Ocean University Center of Excellence for the Oceans National Taiwan Ocean University CAS Key Laboratory for Experimental Study Under Deep-Sea Extreme Conditions Institute of Deep-Sea Science and Engineering Chinese Academy of Sciences CAS-HKUST Sanya Joint Laboratory of Marine Science Research Department of Civil and Environmental Engineering Faculty of Science and Technology Centre for Regional Oceans University of Macau State Key Laboratory of Marine Pollution

Mesoscale eddies are found almost everywhere in global ocean. They can last for weeks to months with scales up to over 100 km and play important roles in global biogeochemical cycles. In this study, we analyzed the phylogenetic and pigment type composition of Synechococcus in a cyclonic eddy (CE, cold eddy) and an anticyclonic eddy (ACE, warm eddy) located in western South China Sea in summer, 2018. Nutrients pumping enhanced Synechococcus abundance markedly in the upper euphotic layers of CE. High diversity of both phylogenetic clades and pigment types of Synechococcus were discovered in the sampling area, with clear composition difference between CE and ACE. The chromatic acclimating pigment type (PT) 3dA dominated in CE while PT 3dB dominated in ACE. The potential weak chromatic acclimator PT 3eA contributed a significant proportion in both CE and ACE. To better understand the difference of PT composition in CE and ACE, we further investigated the phylogenetic composition of Synechococcus in CE and ACE. Clade CRD 1, which were the main strains in upwelling regions, were dominant in CE, where cooler and nutrient rich subsurface water was pumped to the upper layers. Warm water adapted clade II and clade III dominated in ACE. Our study, for the first time, indicated that chromatic acclimation was important in shaping the vertical profile of Synechococcus community in mesoscale eddies of the subtropical oceans. © 2024 The Authors.

关键词： mesoscale eddies phylogenetic composition pigment type South China Sea Synechococcus

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Comparative Effects of Chemical Dispersants and Rhamnolipid Biosurfactants on Oil Biodegradation and Microbial Community Dynamics in Coastal Sediments

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SSRN 2024年

作者： Lu, Lu Deng, Linjie Peng, Chao Li, Shun Yang, Ruiyu Yan, Chenyao Li, Min College of Environmental Science and Engineering China West Normal University Nanchong637009 China College ofLife Sciences China WestNormalUniversity Nanchong637002 China Chemical Synthesis and Pollution Control Key Laboratory of Sichuan Province China WestNormalUniversity Nanchong637009 China State Key Laboratory of Microbial Technology Shandong University PRChina Qingdao266237 China

Marine coastal zones face pollution from both terrestrial and marine petroleum sources. Chemical and biological surfactants are employed to enhance oil dispersal and bioavailability in seawater, yet comparisons of their effects on microbial communities and oil degradation in sediments have not been well documented. Here, we conducted microcosm experiments mimicking oil spill scenarios with coastal sediment from the East China Sea, amended with either a dispersant (Jiefeite or Slickgone NS) or the biosurfactant rhamnolipid. The addition of Jiefeite, Slickgone, and rhamnolipid significantly enhanced oil biodegradation in sediments, with similar effects among them. The enhanced biodegradation activities observed were correlated with increased abundances of phnAc and alkB genes, as well as elevated abundances of predicted functional genes for the degradation of chloroalkane, chloroalkene, benzoates, toluene, and aromatic hydrocarbon. All oil microcosms showed significant growth in Sulfurovum and Woeseia. Oil microcosms treated with Jiefeite or Slickgone specifically enriched potential oil-degraders like Syntrophotalea, Marinobacter, and Sphingomonadaceae. In contrast, rhamnolipid-treated microcosms exhibited increased abundances of oil-degraders such as Pseudomonas, Lachnospirales, Aestuariicella, Vibrio, and Marinobacterium. Our findings underscore the potential of surfactants in enhancing biodegradation and shaping microbial communities, offering insights for emergency coastal oil spill responses. © 2024, The Authors. All rights reserved.

关键词： Microorganisms

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The combined toxicity and mechanism of multi-walled carbon nanotubes and nano zinc oxide toward the cabbage

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environmental science and pollution research international 2022年第3期29卷 3540-3554页

作者： Mo Hong Ji-Lai Gong Wei-Cheng Cao Rong Fang Zhe Cai Jun Ye Zeng-Ping Chen Wang-Wang Tang Key Laboratory of Environmental Biology and Pollution Control (Hunan University) Ministry of Education College of Environmental Science and Engineering Hunan University Changsha 410082 People's Republic of China. Key Laboratory of Environmental Biology and Pollution Control (Hunan University) Ministry of Education College of Environmental Science and Engineering Hunan University Changsha 410082 People's Republic of China. jilaigong@***. Hunan Qing Zhi Yuan Environmental Protection Technology Co. Ltd Changsha 410082 People's Republic of China. State Key Laboratory for Chemo/Biosensing and Chemometrics College of chemistry and Chemical Engineering Hunan University Changsha 410082 People's Republic of China. Key Laboratory of Environmental Biology and Pollution Control (Hunan University) Ministry of Education College of Environmental Science and Engineering Hunan University Changsha 410082 People's Republic of China. wtang@***.

The natural environment is a complex system, and there is never only one kind of nanomaterial entering the environment. However, many studies only considered the plant toxicity of one kind of nanomaterial and do not consider the influence of two or more kinds of nanomaterials on plant toxicity. Multi-walled carbon nanotubes (MWCNTs) and zinc oxide nanoparticles (ZnO NPs) are two common and widely used nanomaterials in water environment, so these two kinds of nanomaterials were chosen to explore the effects of their combined toxicity on cabbage. This study investigated the toxicity of MWCNTs combined with ZnO NPs on cabbage by measuring the length of roots and stems, chlorophyll content, oxidative stress, antioxidant enzyme activity, metal element content, and root scanning electron microscopy. The toxicity of single MWCNTs toward cabbage was attributed to direct oxidative damage, while the toxicity of single ZnO NPs toward cabbage was due to the high level of zinc concentration. Moreover, ZnO NPs (10 mg/L) ameliorated MWCNTs toxicity toward cabbage by improving the activity of antioxidant enzymes. ZnO NPs (50 and 100 mg/L) because of the high content of zinc disrupted the balance of other metals in the plant and increased the toxicity of MWCNTs. In conclusion, the combined toxicity of different concentrations and types of nanomaterials should be considered for a more accurate assessment of environmental risks.

关键词： Cabbage Combined toxicity MWCNTs ZnO NPs

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Carbon flow allocation patterns of CH4, CO2, and biomass production vary with sewage and sediment microbial and biochemical factors in the anaerobic sewer environment

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Chemosphere 2024年 368卷 143744页

作者： Ye, Jianfeng Zhu, Yi Chen, Hao Nie, Yunhan Zhang, Jinxu Chen, Yu Guo, Yali Fang, Ning School of Environmental Science and Engineering Tongji University Shanghai200092 China State Key Laboratory of Pollution Control and Resource Reuse Tongji University Shanghai200092 China Science and Technology Innovation Center for Eco-environmental Protection Shanghai Investigation Design & Research Institute Co. Ltd. Shanghai200050 China YANGTZE Eco-Environment Engineering Research Center Three Gorges Corporation Beijing100038 China Co. Ltd. Shanghai200092 China

Understanding the carbon (C) fate in municipal sewers is imperative for optimizing current sewer-C-degradation control and treatment efficiency, aligning with China's C-neutrality strategy in determining the exact C budget of the wastewater system. This study used laboratory batch tests mimicking the anaerobic sewer environment and sewage-sediment stratification to evaluate C flow allocation (CFA) patterns in response to biotic and abiotic variables. We quantified the C equivalent mass (CEM) and used absolute quantitative 16S rRNA gene amplicon sequencing to characterize the microbiome. The substantial methane production (CH4, 17.2%–18.8%) required both activated sediment and exogenous C, while biomass production (BP, 63.1%–74.9%) formed C sink predominated as the main CFA direction under the stratified state. This was supported by the high diversity, interspecific interactions, and metabolic capacity of the sediment microbiome. However, CH4 and BP patterns demonstrated non-synchronicity and opposite dynamic characteristics. Carbon dioxide (CO2, 64.0%–81.3%) production dominated the sewage CFA. The absolute abundance of the sediment microbiome, which was 5.6 times higher than that of the sewage, exhibited a strong increase in magnitude across the phases. It was primarily associated with biomass growth and N metabolism, whereas sewage showed differentiated and competing communities and appeared to act mainly as the exogenous C sources. We constructed a binary quadratic linear model revealing the non-linear relationship between ACK activity, DOC degradation rate, and CEMCH4 rate;the former maintained low CH4 production when the available substrate was insufficient. The influence of N and S factors on the CFA is complex and multi-faceted. These findings highlight the importance of further investigations into the process-based framework of the sewer C budget, focusing on the C source-emission-sink functions and mass balance. © 2024 Elsevier Ltd

关键词： Carbon sequestration

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Nano-Colloidal Probes to Explore the Bindings between Cellulose Microfibrils and Hemicellulose Assisted with Molecular Dynamics Simulations

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SSRN 2024年

作者： Kong, Yi Lan, Xingyu Zhang, Weixiong Leu, Shao-Yuan Wang, Ying Fu, Shiyu Hu, Chuanshuang State Key Laboratory of Pulp and Paper Engineering South China University of Technology Guangzhou510641 China Faculty of Materials Science and Engineering South China University of Technology Guangzhou510640 China Department of Civil and Environmental Engineering The Hong Kong Polytechnic University 999077 Hong Kong College of Materials and Energy South China Agricultural University Guangzhou510640 China

To interpret the complex interactions between hemicellulose and cellulose may be benefit to the utilization of plant biomass. Herein, a program with AFM colloidal probe technology and molecular dynamics simulations (MD) is attempted to reveal the relationship between cellulose microfibrils and xylan in the cell walls of eucalyptus plants. Two nanocellulose-based colloidal probes were fabricated to measure the intermolecular force between cellulose and xylan. The forces were correlated with the length, diameter, and modifying groups of CNC/CNF, as well as the molecular weight and number of side chains of xylan. MD simulations, while validating the experimental results, suggest that dispersion interactions play an integral role between cellulose microfibers and xylan. These discoveries reveal the underlying principles of polysaccharide interactions behind lignocellulose, providing guidance for the rational design of more readily utilizable plants and more efficient pathways for biomass conversion. © 2024, The Authors. All rights reserved.

关键词： Molecular dynamics

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Activation of Peracetic Acid Via a Hollow Double Layered Co3o4 Polyhedron for the Highly Efficient Removal of Sulfonamides: Kinetics Insights and Assessment of Practical Applications

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SSRN 2022年

作者： Wu, Jianqing Zheng, Xiaoshan Wang, Yingfei Liu, Haijin Wu, Yuliang Jin, Xiaoyu Chen, Ping Lv, Wenying Liu, Guoguang School of Environmental Science and Engineering Guangdong University of Technology Guangzhou510006 China School of Environmental Science and Engineering Guangdong Provincial Key Laboratory of Environmental Pollution Control and Remediation Technology Sun Yatsen University Guangzhou510006 China School of Environment Henan Normal University Key Laboratory for Yellow River and Huaihe River Water Environment and Pollution Control Xinxiang453007 China

Sulfonamides (SAs) have been of ecotoxicological concern for ambient ecosystems due to their widespread application in the veterinary industry. Herein, we developed a powerful advanced oxidation peracetic acid (PAA) activation process for the remediation of SAs with a Co3O4 hollow double-layered structure (Co3O4 HDLSs) catalyst. Systematic characterization results revealed that the polyporous hollow hierarchical structure endows Co3O4 HDLSs with abundant active reaction sites and enhanced mass transfer rate, which were conducive for improving the PAA activation efficiency. Laser flash photolysis experiment and mechanism studies indicated that organic radical species were dominant reactive species for SAs removal. The present system is also highly effective under natural water matrices and trace SAs concentration (20 μg/L) condition. More importantly, the chlorella acute toxicity of the SAs solution was eliminated during mineralization process, supporting this catalytic system may be efficaciously applied for the remediation of SAs contamination in ambient waterways. © 2022, The Authors. All rights reserved.

关键词： Amides

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The effect of hydrostatic pressure on the nitrogen removal potential at the sediment water interface of reservoirs

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Zhongguo Huanjing Kexue/China environmental science 2024年第4期44卷 2119-2129页

作者： Li, Yu-Mei Chen, Kai He, Li-Xin Chai, Bei-Bei Zhuo, Tian-Yu Yu, Ke-Hong Zhang, Jin-Nan Lei, Xiao-Hui School of Water Conservancy and Hydroelectric Power Hebei University of Engineering Handan056038 China School of Water Conservancy and Hydroelectric Hebei University of Engineering Collaborative Innovation Center for Intelligent Regulation and Comprehensive Management of Water Resources Handan056038 China Hebei Key Laboratory of Intelligent Water Conservancy Handan056038 China Handan Key Laboratory of Low-Carbon Energy Handan056038 China Tianjin Water Group Binhai Water Co. Ltd. Tianjin300308 China School of Energy and Environmental Engineering Hebei University of Engineering Handan056038 China School of Architecture and Civil Engineering Xi’an University of Science and Technology Xi′an710054 China State Key Laboratory of Simulation and Regulation of Water Cycle in River Basin China Institute of Water Resources and Hydropower Research Beijing100038 China

The effects of different hydrostatic conditions (atmospheric pressure, 0.2MPa, 0.5MPa and 0.7MPa) on microbial community structure, nitrogen cycling function genes and metabolic pathways at the sediment-water interface of reservoir were studied through microcosmic simulation experiments and metagenomics. The results showed that the number of microbial species involved in nitrogen cycling increased first to 1227 and then decreased to 1199 with the increase of hydrostatic pressure. The relative abundances of archaea and fungi increased by 0.002% and 0.0006% with the increase of hydrostatic pressure, while the proportion of bacteria decreased. High hydrostatic pressure fostered closer ecological network connections, intricate interspecific interactions, and enhanced system stability compared to low pressure. Furthermore, increased hydrostatic pressure facilitated denitrification and repressed dissimilatory nitrate reduction by augmenting the abundance of functional genes such as nxrB and narH, alongside the participating microorganism abundance. Moreover, piezophilic taxa (e.g., Proteobacteria, Chloroflexi, Bacteroidetes) and genes (e.g., ompH, asd) were identified among nitrogen-cycling microorganisms, with a predominant presence in Proteobacteria. Their abundance initially grew and then declined with rising pressure. Hydrostatic pressure can improve the nitrogen removal potential of reservoir sediments by altering the microbial population structure, related functional gene abundance, and metabolic pathways involved in the nitrogen cycle at the sediment-water interface, thereby mitigating reservoir eutrophication. © 2024 Chinese Society for environmental sciences. All rights reserved.

关键词： Microorganisms

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Incorporation of fluoride in calcite: Insights from solid-state NMR, NanoSIMS, APT, HRSTEM and DFT calculations

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Geochimica et Cosmochimica Acta 2025年 401卷 31-46页

作者： Li, Wei Ren, Chao Kwon, Kideok D. Feng, Xiaolei Sha, Gang Li, Jinhui Dong, Sijia Lu, Xiancai Key Laboratory of Surficial Geochemistry Ministry of Education School of Earth Sciences and Engineering Nanjing University Nanjing 210023 China Frontiers Science Center for Critical Earth Material Cycling (FSC-CEMaC) Nanjing University Nanjing 210023 China School of Environmental and Biological Engineering Nanjing University of Science and Technology Nanjing 210094 China Department of Geology Kangwon National University Chuncheon 24347 South Korea School of Materials Science and Engineering Nanyang Technological University 50 Nanyang Avenue Singapore 639798 Singapore School of Materials Science and Engineering/Herbert Gleiter Institute of Nanoscience Nanjing University of Science and Technology Nanjing 210094 China School of Sustainable Energy and Resources Nanjing University Suzhou 215163 China

Despite the abundant occurrence and large variation in fluorine (F) in calcium carbonate minerals in geological settings, it remains poorly understood to what degree F can be incorporated into calcium carbonate minerals. Particularly, molecular-scale evidence for F incorporation modes in the calcite structure is lacking. In this study, we conducted coprecipitation experiments for F with calcium carbonate to reveal the nature of F partitioning in calcite minerals. The ¹⁹F solid-state NMR spectra yield four peaks at −82, −97, −107 and −108 ppm, suggesting that F can be taken up by calcite via at least four mechanisms. The −108 ppm peak occurs at F⁻ concentrations above 2 mM and is consistent with fluorite (CaF2), suggesting that fluorite precipitation predominates at high [F]. Combined with ¹⁹F chemical shifts, ¹⁹F{¹³C} rotational echo double resonance (REDOR) techniques, and DFT-based quantum computations, the ¹⁹F NMR signals at −82, −97 and −107 ppm are assigned to surface adsorbed species, surface incorporated “CaF2” defects and incorporated “CaF2” defects within the bulk of calcite, respectively. Visualization via three-dimensional atomic probe topography (3D APT), high-resolution scanning transmission microscopy (HRSTEM) and nanoscale secondary ion mass spectrometry (NanoSIMS) analysis further supported that F can be incorporated into the bulk structure of calcite. These findings provide atomic and molecular insight into F incorporation in carbonate minerals and are helpful for the application of carbonate materials as potential geochemical proxies.

关键词： APT Calcite Fluoride HRSTEM Incorporation NanoSIMS Solid-state NMR

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