Article
Biotechnology & Applied Microbiology
Brian D. Etz, Manoj K. Shukla
Summary: This paper discusses the elusive challenge of completely and efficiently removing high-profile and chemically diverse PFAS contaminants, and the different degradation strategies that may involve various reaction mechanisms and pathways. The aim of this study is to facilitate the advancement of PFAS destruction methods by elucidating the chemical degradation mechanisms of PFAS.
CURRENT OPINION IN CHEMICAL ENGINEERING
(2023)
Article
Environmental Sciences
Huiming Cao, Jianhua Peng, Zhen Zhou, Yuzhen Sun, Yawei Wang, Yong Liang
Summary: UV-generated hydrated electrons play a critical role in the defluorination reaction of poly- and perfluoroalkyl substances (PFAS). Machine learning algorithms were used to develop predictive models of the relative defluorination ability of PEAS, with gradient boosting algorithms showing superior predictive performance. Electrostatic properties and topological structure significantly affected the defluorination ability of PFAS, with most emerging PEAS being recalcitrant to reductive defluorination.
SCIENCE OF THE TOTAL ENVIRONMENT
(2022)
Article
Engineering, Environmental
Jinhee Park, Shan Huang, Bruce E. Koel, Peter R. Jaffe
Summary: Acidimicrobium sp. Strain A6 can degrade perfluoroalkyl acids (PFAAs) by oxidizing NH4+ while reducing Fe (III). Coating ferrihydrite particles with polyacrylic acid (PAA) with negative surface charge enhanced the Feammox activity and PFOA degradation. This study provides insights into the potential of PAA-coated ferrihydrite for PFAS defluorination.
JOURNAL OF HAZARDOUS MATERIALS
(2023)
Review
Engineering, Environmental
Mohamed Gar Alalm, Daria Camilla Boffito
Summary: This systematic review provides a comprehensive overview of the degradation mechanisms and pathways of perfluoroalkyl substances (PFAS) by various advanced oxidation or reduction processes. The study highlights the importance of the type of reactive oxidant or reductive species in determining the degradation pathways of PFAS. Additionally, the study demonstrates the impact of crystal facets and functional groups on the degradation pathways and defluorination rates when using heterogeneous catalysis.
CHEMICAL ENGINEERING JOURNAL
(2022)
Article
Engineering, Environmental
Jun Sun, Sreenu Jennepalli, Matthew Lee, Adele Jones, Denis M. O'Corroll, Michael J. Mane Field, Mohan Bhadbhade, Bjorn Akermark, Biswanath Das, Naresh Kumar
Summary: Porphyrin-based metal complexes have been found to efficiently degrade PFOS, with higher degradation rate compared to VB12. Moreover, the CoII-TPP-TiIII citrate system can still efficiently degrade PFOS at room temperature.
ENVIRONMENTAL SCIENCE & TECHNOLOGY
(2022)
Article
Chemistry, Physical
Jichao Xiao, John Montgomery
Summary: A simple procedure for the nickel-catalyzed defluorinative alkylation of unactivated aliphatic aldehydes is reported. The protocol exhibits broad substrate scope, mild conditions, and a simple catalytic setup.
Article
Engineering, Environmental
Yangmo Zhu, Haodong Ji, Ke He, Lee Blaney, Tianyuan Xu, Dongye Zhao
Summary: In this study, a novel adsorptive photocatalyst Bi/TNTs@AC was developed for efficient adsorption and solid-phase photodegradation of GenX. The material mainly consists of activated carbon, anatase, and bismuth nanoparticles with a metallic bismuth core covered by an amorphous Bi2O3 shell. Through analysis and calculations, it was found that Bi/TNTs@AC can degrade GenX into shorter-chain fluorinated compounds through a stepwise defluorination mechanism. The results suggest that Bi/TNTs@AC holds potential for more cost-effective degradation of GenX.
Article
Engineering, Environmental
Bosen Jin, Yiwen Zhu, Weiyang Zhao, Zekun Liu, Shun Che, Kunpeng Chen, Ying-Hsuan Lin, Jinyong Liu, Yujie Men
Summary: This study investigated the structure-biodegradability relationship for different ether PFAS in activated sludge communities. Only polyfluorinated ethers with specific molecular structures underwent biotransformation, leading to the formation of unstable fluoroalcohol intermediates subject to spontaneous defluorination. The findings suggest that aerobic biotransformation/defluorination can complement advanced reduction processes for cost-effective treatment of PFAS.
ENVIRONMENTAL SCIENCE & TECHNOLOGY LETTERS
(2023)
Article
Environmental Sciences
Conrad Austin, Jianna Li, Stuart Moore, Anmol Purohit, Brian R. Pinkard, Igor Novosselov
Summary: Cleanup and disposal of stockpiles and waste streams containing per- and polyfluoroalkyl substances (PFAS) require effective end-of-life destruction/mineralization technologies. Continuous flow supercritical water oxidation (SCWO) reactors have been shown to effectively destroy PFAS compounds. However, the comparison between the efficacy of SCWO treatment on PFSAs and PFCAs has not been reported.
Review
Environmental Sciences
Ashenafi Berhanu, Ishmael Mutanda, Ji Taolin, Majjid A. Qaria, Bin Yang, Daochen Zhu
Summary: Since the 1950s, large amounts of PFAS have been dumped into the environment, causing significant contamination. PFAS are resistant to degradation and have adverse effects on health and the environment. Traditional physicochemical methods for PFAS treatment have drawbacks, making microbial degradation and enzymatic treatment highly sought after. This review provides an overview of PFAS classification, properties, and interaction with the environment, and discusses recent developments in microbial degradation, transformation routes, and challenges in bioremediation approaches.
SCIENCE OF THE TOTAL ENVIRONMENT
(2023)
Article
Environmental Sciences
Brian R. Pinkard, Shreyas Shetty, Derek Stritzinger, Christopher Bellona, Igor Novosselov
Summary: Effective technologies, such as supercritical water oxidation (SCWO), are needed for the destruction of PFAS. This study found that destruction and defluorination efficiencies of PFOS via SCWO were influenced by temperature and residence time, with a maximum 70.0% PFOS destruction and 78.2% defluorination achieved at 500 degrees C after 60 minutes of reaction.
Article
Environmental Sciences
Valentina Mendez, Sophie Holland, Shefali Bhardwaj, James McDonald, Stuart Khan, Denis O'Carroll, Russell Pickford, Sarah Richards, Casey O'Farrell, Nicholas Coleman, Matthew Lee, Michael J. Manefield
Summary: In this study, a bacterial strain capable of utilizing 6:2 FTS as a sulfur source was isolated and analyzed for its genomic and proteomic characteristics. The findings provide insights into the biodegradation of 6:2 FTS by the Actinobacterium D. aurantiaca J3, informing the fate of PFAS in the environment.
SCIENCE OF THE TOTAL ENVIRONMENT
(2022)
Article
Engineering, Environmental
Danielle R. Schlesinger, Collin McDermott, Nam Q. Le, Jesse S. Ko, James K. Johnson, Plamen A. Demirev, Zhiyong Xia
Summary: Finding economically-sustainable and environmentally-friendly technologies for PFAS destruction is crucial due to the increasing contamination of PFAS in drinking water globally. UV-Fenton chemistry, catalyzed by nanosize magnetite particles, shows promising results in generating ROS, which can disrupt PFAS carbon-fluorine bonds.
ENVIRONMENTAL SCIENCE-WATER RESEARCH & TECHNOLOGY
(2022)
Article
Biotechnology & Applied Microbiology
Madison D. Bygd, Kelly G. Aukema, Jack E. Richman, Lawrence P. Wackett
Summary: Thousands of organofluorine chemicals are known to be persistent and toxic environmental pollutants, but few bacteria biodegrade fluorinated chemicals. A rapid screening method was developed to discover new organofluoride biodegradation, revealing 21 new microbial defluorination reactions. A general mechanism was delineated for the biodegradation of trifluoromethylphenyl groups that are increasingly being used in drugs and pesticides.
APPLIED AND ENVIRONMENTAL MICROBIOLOGY
(2022)
Review
Engineering, Environmental
Rebecca A. Dickman, Diana S. Aga
Summary: The fate, effects, and treatment of per- and polyfluoroalkyl substances (PFAS) are of great interest due to their widespread presence in the environment and significant toxicological effects on humans and wildlife. This article reviews selected papers from the Journal of Hazardous Materials on the toxicity, sequestration, and degradation of PFAS, and makes them available as open-access publications to facilitate the distribution of critical knowledge on PFAS. The review discusses routes of toxicity, observed human health effects, in-silico approaches for toxicity evaluation, removal methods, and degradation techniques for PFAS.
JOURNAL OF HAZARDOUS MATERIALS
(2022)
Article
Chemistry, Multidisciplinary
Peigen Liu, Zixiang Huang, Xiaoping Gao, Xun Hong, Junfa Zhu, Gongming Wang, Yuen Wu, Jie Zeng, Xusheng Zheng
Summary: This study demonstrates the synergistic function between single Pd atoms and Pd nanoparticles on graphitic carbon nitride for selective photocatalytic reduction of CO2 into CH4, providing a new perspective for the development of selective photocatalytic CO2 conversion.
ADVANCED MATERIALS
(2022)
Article
Chemistry, Physical
Xuejiao Sun, Cai Chen, Can Xiong, Congmin Zhang, Xusheng Zheng, Jin Wang, Xiaoping Gao, Zhen-Qiang Yu, Yuen Wu
Summary: Single atom catalysts have great potential in the fabrication of electrochemical biosensors due to their unexpected catalytic selectivity and activity. In this study, a highly sensitive dopamine sensor was designed and fabricated using flower-like MoS2 decorated with a single Ni site catalyst. The sensor exhibited excellent performance with low detection limits in various solutions. The exceptional sensing capabilities can be attributed to the axial anchoring of Ni single atoms on the MoS2 basal plane.
Article
Chemistry, Multidisciplinary
Congmin Zhang, Lichen Bai, Min Chen, Xuejiao Sun, Mengzhao Zhu, Qinglong Wu, Xiaoping Gao, Qun Zhang, Xusheng Zheng, Zhen-Qiang Yu, Yuen Wu
Summary: The site density of Mo single atoms on RPCN is controlled by a local carbonization strategy, capturing adventitious O atoms and forming O-covered Mo-N-3 coordination. Coordinated O atoms create a catalytic environment with Lewis base and gather photo-generated electrons under light. The resulting Mo-RPCN exhibits a strong ability for hydrogen abstraction.
ADVANCED MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Wenxin Guo, Xiaoping Gao, Mengzhao Zhu, Chenxi Xu, Xiaorong Zhu, Xuyan Zhao, Rongbo Sun, Zhenggang Xue, Jia Song, Lin Tian, Jie Xu, Wenxing Chen, Yue Lin, Yafei Li, Huang Zhou, Yuen Wu
Summary: A gas-promoted dealloying process was reported to prepare a hybrid electrocatalyst containing Pt-based alloy nanocrystals and dense isolated Ni sites. The resulting catalyst exhibits excellent oxygen reduction reaction (ORR) activity and greatly reduces the usage of Pt.
ENERGY & ENVIRONMENTAL SCIENCE
(2023)
Article
Chemistry, Physical
Xiaoping Gao, Huang Zhou, Zhe Wang, Gang Zhou, Jin Wang, Yuen Wu
Summary: This study systematically investigates the stability and OER activity of several antimonate-based electrocatalysts under acidic conditions, and identifies some efficient and stable catalysts with better OER catalytic activities than the current state-of-the-art catalyst (IrO2). These findings highlight the potential of antimonate-based OER electrocatalysts for future experimental verification.
Article
Chemistry, Multidisciplinary
Xiaole Zhao, Geng Wu, Xusheng Zheng, Peng Jiang, Jun-dong Yi, Huang Zhou, Xiaoping Gao, Zhen-Qiang Yu, Yuen Wu
Summary: Charge redistribution on the surface of Ru nanoparticle greatly affects the electrocatalytic HER activity. A double atomic-tuned RuBi SAA/Bi@OG nanostructure, consisting of RuBi single-atom alloy nanoparticle supported by Bi-O single-site-doped graphene, was successfully developed. The synergy between the alloyed Bi single atom and adjacent Bi-O single site in RuBi SAA/Bi@OG effectively manipulates electron transfer on the Ru surface, resulting in optimal charge redistribution and superior alkaline HER activity.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Immunology
Jianwen Wu, Jing Xiao, Min Bai, Chunli Shi, Yunzhuo Xin, Wei Zhao, Xiaoping Gao, Mei Yin, Jiaqing Zhao
Summary: This study used single-cell RNA sequencing and immunome repertoire sequencing to analyze immune cell changes in mice infected with Echinococcus granulosus. The results showed tissue-specific alterations in the immune system, including the induction of specific CD4(+) cells and the presence of different Treg cell subpopulations. These findings contribute to a better understanding of the immunomodulatory mechanisms in E. granulosus infection.
INFECTION AND IMMUNITY
(2023)
Article
Engineering, Environmental
Zhan-Chao Li, Wei Li, Rui Wang, Dong-Xia Wang, An-Na Tang, Xiao-Peng Wang, Xiao-Ping Gao, Gai-Ming Zhao, De -Ming Kong
Summary: In this study, a new type of green lignin-based covalent organic polymers (LIGOPD-COPs) were successfully fabricated with lignin and water as the raw material and reaction solvent, respectively. The LIGOPD-COPs exhibited improved crystallinity compared to previous lignin-based polymers, leading to enhanced application performance in non-targeted food safety analysis.
JOURNAL OF HAZARDOUS MATERIALS
(2023)
Article
Chemistry, Physical
Wenxin Guo, Liming Cheng, Xiaoping Gao, Jie Xu, Cai Chen, Peigen Liu, Dayin He, Lin Tian, Jia Song, Huang Zhou, Yuen Wu
Summary: In this study, a highly efficient 3D hierarchical porous oxygen reduction reaction (ORR) catalytic system was developed by incorporating stable and multiaperture zirconia (ZrO2) and conductive N-doped carbon (NC) into a Pt-based catalyst. The Pt-ZrO2 interface greatly enhances the activation of O2, while the hierarchical porous structure of a NC-encapsulated nanoframework promotes mass diffusion and electron transfer, leading to improved ORR activity and stability. This catalytic system exhibits significantly higher mass activity/specific activity than commercial Pt/C, and shows negligible activity decay and morphological stability after long-term cycling. The integration of hierarchical porous systems for optimizing the geometric and electric structure of Pt-based catalysts has great potential for practical proton exchange membrane fuel cells (PEMFCs).
Article
Microbiology
Ruosong Qu, Guanzhen Liu, Ming Yue, Gangsheng Wang, Changhui Peng, Kefeng Wang, Xiaoping Gao
Summary: Soil microorganisms are important indicators for evaluating soil health and their role in carbon-climate feedback is vital. This study conducted an observational experiment in the Ziwuling Mountains, Loess Plateau, China, and found that soil respiration rate is significantly correlated with temperature and moisture, indicating that temperature increase leads to soil carbon loss. The study also revealed the crucial factors affecting soil microbial activity and provided valuable scientific implications for constructing microbial decomposition models to predict soil microbial activity under climate change in the future.
FRONTIERS IN MICROBIOLOGY
(2023)
Review
Engineering, Environmental
Jiaxin Zhu, Zekun Liu, Yihua Chen, Zhiqiang Chen, Hang Ma, Jian Sun, Liao Meng, Tongzhou Liu
Summary: The discharge of widely used fluorinated aromatics (FAs) leads to their notoriously high persistence and toxicity in natural environments. Defluorination is the key step for FAs pollutants detoxification. In this study, 4-fluorophenol (4-FP) was selected as a model compound to optimize the electrochemical hydrodefluorination (HDF) process and understand the reaction mechanism. The investigation showed that Rh coating outperformed Pd coating due to its higher reactivity towards C-F bond cleavage.
CHEMICAL ENGINEERING JOURNAL
(2023)
Article
Multidisciplinary Sciences
Qiuping Wang, Kui Chen, Hui Jiang, Cai Chen, Can Xiong, Min Chen, Jie Xu, Xiaoping Gao, Suowen Xu, Huang Zhou, Yuen Wu
Summary: This study presents a design of biomimetic cascade catalysis system, where metal sites are immobilized on the inner and outer layers of nanocapsules to enable efficient enzymatic cascade reactions. The biomimetic catalysis system exhibits higher activity enhancement compared to conventional systems and is successfully applied in glucose detection.
NATURE COMMUNICATIONS
(2023)
Article
Chemistry, Physical
Zhenggang Xue, Xiaoping Gao, Yida Zhang, Muyu Yan, Jiaqiang Xu, Yuen Wu
Summary: Engineering the site density of single-atom catalysts (SACs) on a confined catalyst surface can improve catalytic performances. We demonstrate an optimal single Pt site coverage (about 0.34 Pt/nm2) over a CdS-confined Pt single-atom-layer surface for effective hydrogen evolution. The interactions between overly dense Pt monomers deteriorate the adsorption and desorption behaviors of hydrogen.
Article
Chemistry, Physical
Wenxin Guo, Liming Cheng, Xiaoping Gao, Jie Xu, Cai Chen, Peigen Liu, Dayin He, Lin Tian, Jia Song, Huang Zhou, Yuen Wu
Summary: In this work, a highly efficient 3D hierarchical porous oxygen reduction reaction (ORR) catalytic system was developed by introducing stable and multiaperture zirconia (ZrO2) and conductive N-doped carbon (NC) into a Pt-based catalyst. The Pt-ZrO2 interface greatly enhanced the activation of O2 by modulating the electronic state of Pt nanoparticles. The hierarchical porous structure of a NC-encapsulated nanoframework compensated for system conductivity, promoting mass diffusion and electron transfer, thus enhancing the ORR activity and stability.
Article
Chemistry, Physical
Muyu Yan, Xiaoping Gao, Xiao Han, Danni Zhou, Yue Lin, Wenxing Chen, Zhenggang Xue, Yuen Wu
Summary: Researchers created gas-microchannels on TiO2 nanorod-supported Pt single-atom catalyst to guide and transfer reactant molecules to achieve high-efficient reactions. The final Pt-1/TiO2 catalysts showed a high sensing response to acetone gas, approximately three times higher than catalysts without scaly shell.