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Direct Conversion of N2 to Nitric Acid via Contact Electrocatalysis SCIE
期刊论文 | 2025 , 13 (27) , 10486-10494 | ACS SUSTAINABLE CHEMISTRY & ENGINEERING
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Abstract :

Nitric acid (HNO3) as a vital chemical is widely used in energy and environmental fields. However, its conventional production relies on ammonia synthesis, resulting in high energy consumption and environmental concerns. Here, we report a simple, efficient, and green conversion of N2 to HNO3 by contact electrocatalysis (CEC) under ambient conditions. Utilizing the electrification of poly(tetrafluoroethylene) (PTFE) particles with water under ultrasound, we demonstrate how this interaction promotes the activation of N2. Our results showed that the average yield of HNO3 can reach 40.73 +/- 1.80 mu M h-1 in air gas atmosphere. We utilized electron spin resonance and the fluorescence spectrum to confirm the evolution of hydroxyl radicals (OH). High-resolution mass spectrometry combined with isotope experiments provides strong evidence that water-PTFE can produce a contact electric effect through ultrasonic treatment, directly oxidize water or reduce O2 to produce OH, and oxidize N2 to produce HNO3 under anaerobic or aerobic conditions. This work not only provides a green and efficient method for direct N2 fixation into HNO3 but also stimulates further exploration of CEC-driven chemical processes, particularly highlighting its potential for industrial application, and attempts to explain some of the N2 fixation phenomena in the environment.

Keyword :

contact electrocatalysis (CEC) contact electrocatalysis (CEC) hydroxyl radicals hydroxyl radicals nitric acid nitric acid nitrogen nitrogen poly(tetrafluoroethylene)(PTFE) poly(tetrafluoroethylene)(PTFE) water oxidation water oxidation

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GB/T 7714 Huang, Shaofu , Liu, Yuhui , Ren, Lincong et al. Direct Conversion of N2 to Nitric Acid via Contact Electrocatalysis [J]. | ACS SUSTAINABLE CHEMISTRY & ENGINEERING , 2025 , 13 (27) : 10486-10494 .
MLA Huang, Shaofu et al. "Direct Conversion of N2 to Nitric Acid via Contact Electrocatalysis" . | ACS SUSTAINABLE CHEMISTRY & ENGINEERING 13 . 27 (2025) : 10486-10494 .
APA Huang, Shaofu , Liu, Yuhui , Ren, Lincong , Huang, Lingyan , Tang, Jiahuan , Yu, Zhen et al. Direct Conversion of N2 to Nitric Acid via Contact Electrocatalysis . | ACS SUSTAINABLE CHEMISTRY & ENGINEERING , 2025 , 13 (27) , 10486-10494 .
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Non-radical activation of peroxymonosulfate by iron-chitosan carbonization composites for selective bisphenol A degradation: Focusing on singlet oxygen and iron-oxo species SCIE
期刊论文 | 2025 , 40 | ENVIRONMENTAL TECHNOLOGY & INNOVATION
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Abstract :

The contamination of emerging organic contaminants (EOCs) in natural waters poses a serious threat to environmental and public health. Advanced oxidation processes (AOPs) based on non-radical reactive species are considered the mainstream methods for degrading EOCs. However, the catalysts used for oxidant activation often suffer from elaborate synthesis, poor stability and low selectivity. Herein, a one-pot carbonization of chitosan-FeCl3 complexes was designed to yield Fe/Fe3O4-embedded graphitic carbon (FC900) catalyst. This catalyst was capable of activating peroxymonosulfate (PMS) for selective degradation of bisphenol A (BPA). The FC900/PMS system removed 97.8 % BPA within 40 min with a rate constant k of 0.09 min(-1), which was nine times faster than that by nano-Fe3O4/PMS. Singlet oxygen and high-valent iron-oxo species were identified as the primary reactive species with negligible center dot OH/SO4-center dot contribution, demonstrating a non-radical reactive species-dominated degradation process. The system showed excellent tolerance to interference from common anions and natural organic matter, and could be reused for five cycles. It achieved an oxidant utilization efficiency of 0.33 mg BPA per mg PMS, among the best surveyed PMS activator systems to date. The results provide insight into developing simple, stable and efficient catalysts for the treatment of EOCs in complex environment.

Keyword :

Chitosan-derived carbon Chitosan-derived carbon High-valent iron-oxo High-valent iron-oxo Non-radical oxidation Non-radical oxidation Peroxymonosulfate Peroxymonosulfate Singlet oxygen Singlet oxygen

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GB/T 7714 Li, Yang , Yu, Yuqing , Diao, Youming et al. Non-radical activation of peroxymonosulfate by iron-chitosan carbonization composites for selective bisphenol A degradation: Focusing on singlet oxygen and iron-oxo species [J]. | ENVIRONMENTAL TECHNOLOGY & INNOVATION , 2025 , 40 .
MLA Li, Yang et al. "Non-radical activation of peroxymonosulfate by iron-chitosan carbonization composites for selective bisphenol A degradation: Focusing on singlet oxygen and iron-oxo species" . | ENVIRONMENTAL TECHNOLOGY & INNOVATION 40 (2025) .
APA Li, Yang , Yu, Yuqing , Diao, Youming , Li, Yixi , Xie, Zihan , Chen, Man . Non-radical activation of peroxymonosulfate by iron-chitosan carbonization composites for selective bisphenol A degradation: Focusing on singlet oxygen and iron-oxo species . | ENVIRONMENTAL TECHNOLOGY & INNOVATION , 2025 , 40 .
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Natural electricity production from soil-air water exchange: A wide and untapped energy SCIE
期刊论文 | 2025 , 135 | NANO ENERGY
WoS CC Cited Count: 4
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Abstract :

The exchange of water between soil and air is a ubiquitous natural phenomenon. Evaporation and condensation are the two main processes that extract or release energy from the environment. However, due to the low energy density and complex interface of soil, the associated energy has long been overlooked and under-exploited. Here we demonstrate that the energy can be converted into electricity in situ through the hydrovoltaic effect within the soil itself. The soil-based hydrovoltaic electricity generators exhibit excellent reproducibility and stability, demonstrating the potential for scalable integration. A series voltage of over 13.4 V was achieved, placing it in the top five of integrated devices reported to date. By designing an integrated module suitable for amplifying natural electricity from both soil evaporation and soil condensation process, a parallel current of up to 18.62 mu A (0.06 m2) was obtained. The availability of soil demonstrates the great potential of the soil-based electricity generators. This finding demonstrates a green and sustainable technology for electricity generation, and points to possible biogeochemical processes due to the hydrovoltaic effect of soil.

Keyword :

Evaporation-induced electricity generation Evaporation-induced electricity generation Hydrovoltaic effect Hydrovoltaic effect Moisture-induced electricity generation Moisture-induced electricity generation Soil-air water exchange Soil-air water exchange Soil electricity generation Soil electricity generation

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GB/T 7714 Diao, Youming , Hu, Qichang , Liu, Yingying et al. Natural electricity production from soil-air water exchange: A wide and untapped energy [J]. | NANO ENERGY , 2025 , 135 .
MLA Diao, Youming et al. "Natural electricity production from soil-air water exchange: A wide and untapped energy" . | NANO ENERGY 135 (2025) .
APA Diao, Youming , Hu, Qichang , Liu, Yingying , Zeng, Raymond Jianxiong , Zhou, Shungui , Chen, Man . Natural electricity production from soil-air water exchange: A wide and untapped energy . | NANO ENERGY , 2025 , 135 .
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A scalable photovoltaic-type photoelectrotrophic denitrification reactor for selective conversion nitrate to nitrogen via isolating reactive oxygen species SCIE
期刊论文 | 2025 , 507 | CHEMICAL ENGINEERING JOURNAL
WoS CC Cited Count: 1
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Abstract :

Photoelectrotrophic denitrification (PEDeN) is an innovative denitrification process with great potential for nitrate (NO3-) removal from carbon-deficient wastewater. However, the inevitable presence of reactive oxygen species (ROS) significantly undermines the sustainability of PEDeN, including inducing substantial nitrous oxide (N2O) accumulation and declining system's performance. This work demonstrates a proof-of-principle of a photovoltaic (PV)-type PEDeN reactor, where the dominant ROS, including hydrogen peroxide and hydroxyl radicals, are completely isolated from denitrifiers. This way enabled NO3- to be selectively reduced (100%) to nitrogen with minimal N2O emission. The maximum accumulated N2O-N relative to input NO3--N was 11.3%, significantly lower than that in hybrid systems, such as Thiobacillus denitrificans-CdS (72.1%) and Thiobacillus denitrificans-AQS (95.5%). After eliminating ROS, the NO3- removal efficiency in each cyclic experiment reached 100% and the nitrogenous intermediators, such as nitrite and N2O, could be minimized via enhancing the photocurrent. Importantly, NO3- reduction continued even when no chemicals was added, indicating that water can serve as the end electron donor. This study introduces a PV-type PEDeN reactor concept for sustainable nitrate removal via mitigating the toxic effects of ROS and it will offer a cost-effective, environmentally friendly, and scalable technology for removing NO3- pollutants from carbon-deficient wastewater.

Keyword :

Carbon-deficient wastewater Carbon-deficient wastewater Nitrate reduction Nitrate reduction Nitrous oxide emission Nitrous oxide emission Photoelectrotrophic denitrification Photoelectrotrophic denitrification Reactive oxygen species Reactive oxygen species

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GB/T 7714 Chen, Man , Chen, Keyan , Li, Yang et al. A scalable photovoltaic-type photoelectrotrophic denitrification reactor for selective conversion nitrate to nitrogen via isolating reactive oxygen species [J]. | CHEMICAL ENGINEERING JOURNAL , 2025 , 507 .
MLA Chen, Man et al. "A scalable photovoltaic-type photoelectrotrophic denitrification reactor for selective conversion nitrate to nitrogen via isolating reactive oxygen species" . | CHEMICAL ENGINEERING JOURNAL 507 (2025) .
APA Chen, Man , Chen, Keyan , Li, Yang , Diao, Youming , Li, Yixi , Zeng, Raymond Jianxiong et al. A scalable photovoltaic-type photoelectrotrophic denitrification reactor for selective conversion nitrate to nitrogen via isolating reactive oxygen species . | CHEMICAL ENGINEERING JOURNAL , 2025 , 507 .
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Uncovering the Nonnegligible Mechanism of Degrading Structural Extracellular Polymeric Substances for Nitrate Removal in Psychrophilic (15 degree celsius) Waste-Activated Sludge Fermentation ESCI
期刊论文 | 2024 , 4 (5) , 2270-2280 | ACS ES&T WATER
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Wastewater treatment plants (WWTPs) are being challenged to operate as carbon-neutral and energy-efficient systems. The structural extracellular polymeric substances (St-EPS) in waste-activated sludge (WAS), such as alginate, were revealed to form an architectural gel matrix, hindering the psychrophilic hydrolysis and acidogenesis and its application in nitrate removal. Consequently, volatile fatty acid (VFAs) production for nitrate removal at 15 degree celsius is demonstrated by a novel, enriched psychrophilic consortium for alginate-degrading and nitrate-removing. Both alginate lyase (EC 4.2.2.3) and oligo-alginate lyase (EC 4.2.2.26) are identified for alginate utilization by the metaproteomics analysis. A high nitrate removal rate of 7.6 (WAS as the substrate) to 13.0 (alginate as the substrate) mgN/(gVSS h) was achieved. By combining high-throughput and PacBio sequencing and metagenomics analysis, two genera of Bacteroides (69.4%) and Dysgonomons (12.8%) are revealed to enhance psychrophilic WAS fermentation. The VFAs can be utilized by denitrifiers for nitrate removal in an indirect pathway. Moreover, other genera of denitrifiers (Pseudomonas, 0.11%; and Massilla, 0.003%) can excrete alginate lyase, indicating the dual merits of St-EPS degradation and nitrate removal in the direct pathway. This work extends the application of WAS for denitrifiers, providing a new carbon-neutral and energy-efficient system in WWTPs, especially under psychrophilic conditions.

Keyword :

metagenomics metagenomics metaproteomics metaproteomics nitrate removal nitrate removal psychrophilic consortium of alginate-degrading and nitrate-removing psychrophilic consortium of alginate-degrading and nitrate-removing structural extracellular polymeric substances structural extracellular polymeric substances waste-activatedsludge waste-activatedsludge

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GB/T 7714 Wang, Yi-Bo , Tang, Jie , Yan, Yang et al. Uncovering the Nonnegligible Mechanism of Degrading Structural Extracellular Polymeric Substances for Nitrate Removal in Psychrophilic (15 degree celsius) Waste-Activated Sludge Fermentation [J]. | ACS ES&T WATER , 2024 , 4 (5) : 2270-2280 .
MLA Wang, Yi-Bo et al. "Uncovering the Nonnegligible Mechanism of Degrading Structural Extracellular Polymeric Substances for Nitrate Removal in Psychrophilic (15 degree celsius) Waste-Activated Sludge Fermentation" . | ACS ES&T WATER 4 . 5 (2024) : 2270-2280 .
APA Wang, Yi-Bo , Tang, Jie , Yan, Yang , Hong, Si-Di , Zheng, Si-Jie , Huang, Xing-Chen et al. Uncovering the Nonnegligible Mechanism of Degrading Structural Extracellular Polymeric Substances for Nitrate Removal in Psychrophilic (15 degree celsius) Waste-Activated Sludge Fermentation . | ACS ES&T WATER , 2024 , 4 (5) , 2270-2280 .
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Biophotoelectrochemistry for the treatment of emerging contaminants SCIE
期刊论文 | 2024 , 67 (10) , 3051-3066 | SCIENCE CHINA-TECHNOLOGICAL SCIENCES
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Emerging contaminants (ECs) of significant concern are widely distributed throughout the environment due to various industrial practices and human activities. Given the alarming ecological threats and potential risks that ECs pose to human health and aquatic life, even at trace concentrations, it is imperative to develop innovative technologies to effectively address these challenges. The biophotoelectrochemistry (BPEC) system, which integrates microbial cells with photosensitizers for solar-to-chemical conversion, holds great potential as an efficient strategy for the removal of ECs. In this review, we provide new insights into the BPEC system for the ECs treatment by systematically summarizing the classification, sources, and environmental occurrence of ECs. Additionally, we explore the research progress and degradation mechanisms in ECs removal with BPEC. Finally, the current challenges and future perspectives for the applications of the BPEC system in the ECs treatment are analyzed. This review aims to promote the development of BPEC technology for ECs treatment, offering a promising prospect for environmental remediation, circular economy, and clean-energy production.

Keyword :

biodegradation biodegradation biophotoelectrochemistry biophotoelectrochemistry emerging contaminants emerging contaminants photocatalysis photocatalysis

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GB/T 7714 Hu, Jing , Chen, Man , Gu, Wenzhi et al. Biophotoelectrochemistry for the treatment of emerging contaminants [J]. | SCIENCE CHINA-TECHNOLOGICAL SCIENCES , 2024 , 67 (10) : 3051-3066 .
MLA Hu, Jing et al. "Biophotoelectrochemistry for the treatment of emerging contaminants" . | SCIENCE CHINA-TECHNOLOGICAL SCIENCES 67 . 10 (2024) : 3051-3066 .
APA Hu, Jing , Chen, Man , Gu, Wenzhi , Deng, Wener , Hong, Mingqiu , Hu, Andong et al. Biophotoelectrochemistry for the treatment of emerging contaminants . | SCIENCE CHINA-TECHNOLOGICAL SCIENCES , 2024 , 67 (10) , 3051-3066 .
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Interspecies ecological competition rejuvenates decayed Geobacter electroactive biofilm SCIE
期刊论文 | 2024 , 18 (1) | ISME JOURNAL
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Bioelectrochemical systems (BESs) exploit electroactive biofilms (EABs) for promising applications in biosensing, wastewater treatment, energy production, and chemical biosynthesis. However, during the operation of BESs, EABs inevitably decay. Seeking approaches to rejuvenate decayed EABs is critical for the sustainability and practical application of BESs. Prophage induction has been recognized as the primary reason for EAB decay. Herein, we report that introducing a competitive species of Geobacter uraniireducens suspended prophage induction in Geobacter sulfurreducens and thereby rejuvenated the decayed G. sulfurreducens EAB. The transcriptomic profile of G. sulfurreducens demonstrated that the addition of G. uraniireducens significantly affected the expression of metabolism- and stress response system-related genes and in particular suppressed the induction of phage-related genes. Mechanistic analyses revealed that interspecies ecological competition exerted by G. uraniireducens suppressed prophage induction. Our findings not only reveal a novel strategy to rejuvenate decayed EABs, which is significant for the sustainability of BESs, but also provide new knowledge for understanding phage-host interactions from an ecological perspective, with implications for developing therapies to defend against phage attack. Graphical Abstract

Keyword :

bioelectrochemical system bioelectrochemical system biofilm decay biofilm decay ecological competition ecological competition electroactive biofilm electroactive biofilm Geobacter species Geobacter species prophage induction prophage induction

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GB/T 7714 Ye, Yin , Zhang, Lu , Hong, Xiaohui et al. Interspecies ecological competition rejuvenates decayed Geobacter electroactive biofilm [J]. | ISME JOURNAL , 2024 , 18 (1) .
MLA Ye, Yin et al. "Interspecies ecological competition rejuvenates decayed Geobacter electroactive biofilm" . | ISME JOURNAL 18 . 1 (2024) .
APA Ye, Yin , Zhang, Lu , Hong, Xiaohui , Chen, Man , Liu, Xing , Zhou, Shungui . Interspecies ecological competition rejuvenates decayed Geobacter electroactive biofilm . | ISME JOURNAL , 2024 , 18 (1) .
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集成式微生物光电化学反应器处理缺碳废水硝酸盐的方法 ipsunlight
专利 | 2023-11-21 | CN202311557652.0
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本发明公开了一种集成式微生物光电化学反应器处理缺碳废水硝酸盐的新方法,该方法将化学性质稳定,无毒、光催化活性高等优点纳米半导体材料TiO2和Thiobacillus denitrificans生物膜系统耦合构成无机半导体‑微生物体系;在光照条件下Thiobacillus denitrificans生物膜利用光生电子将NO3‑还原为N2。本发明克服了传统无机半导体与微生物结合的操作过程复杂、光照产生的活性氧损伤细菌,降低量子效率和抑制氧化亚氮还原酶(NOS),从而产生大量温室气体(N2O)等缺点;具有工艺简单、能耗低、环保经济和安全可靠的优点,且系统构造相对简单,使其更易于以模块化方式进行修改和改进,因此可进行大规模的推广应用。

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GB/T 7714 陈曼 , 陈柯言 , 周顺桂 . 集成式微生物光电化学反应器处理缺碳废水硝酸盐的方法 : CN202311557652.0[P]. | 2023-11-21 .
MLA 陈曼 et al. "集成式微生物光电化学反应器处理缺碳废水硝酸盐的方法" : CN202311557652.0. | 2023-11-21 .
APA 陈曼 , 陈柯言 , 周顺桂 . 集成式微生物光电化学反应器处理缺碳废水硝酸盐的方法 : CN202311557652.0. | 2023-11-21 .
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基于生物合成的四氧化三锰纳米酶及其减排土壤N2O的应用 ipsunlight
专利 | 2023-11-17 | CN202311542661.2
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本发明公开了基于生物合成的四氧化三锰纳米酶及其减排土壤N2O的应用,本方案能够以土壤中丰富的微生物资源——Escherichia coli作为载体,利用植物微量元素肥料成分中的MnCl2·4H2O,进行简单的生物化学反应,在其表面合成具有酶活性的纳米级矿物Mn3O4,通过淬灭土壤反硝化过程中产生的活性氧来保证Nos的酶活性,使N2O高效还原为N2,促进土壤N2O减排。本发明克服了传统生产过程中工艺复杂、成本高等问题,具有合成工艺简单、绿色经济的、产物酶活性较高、环境风险较低的优点。系统的相对简单性使得它们更易于以模块化方式进行修改和改进,因此可进行大规模的推广应用。

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GB/T 7714 陈曼 , 杨景 , 周顺桂 . 基于生物合成的四氧化三锰纳米酶及其减排土壤N2O的应用 : CN202311542661.2[P]. | 2023-11-17 .
MLA 陈曼 et al. "基于生物合成的四氧化三锰纳米酶及其减排土壤N2O的应用" : CN202311542661.2. | 2023-11-17 .
APA 陈曼 , 杨景 , 周顺桂 . 基于生物合成的四氧化三锰纳米酶及其减排土壤N2O的应用 : CN202311542661.2. | 2023-11-17 .
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Harnessing microbes to pioneer environmental biophotoelectrochemistry SCIE
期刊论文 | 2024 , 42 (12) , 1677-1690 | TRENDS IN BIOTECHNOLOGY
WoS CC Cited Count: 7
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In seeking sustainable environmental strategies, microbial biophotoelectrochemistry (BPEC) systems represent a significant advancement. In this review, we underscore the shift from conventional bioenergy systems to sophisticated BPEC applications, emphasizing their utility in leveraging solar energy for essential biochemical conversions. Recent progress in BPEC technology has facilitated improved photoelectron transfer and system stability, resulting in substantial advancements in carbon and nitrogen fixation, degradation of pollutants, and energy recovery from wastewater. Advances in system design and synthetic biology have expanded the potential of BPEC for environmental clean-up and sustainable energy generation. We also highlight the challenges of environmental BPEC systems, ranging from performance improvement to future applications.

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GB/T 7714 Huang, Shaofu , Ye, Jie , Gao, Jiangtao et al. Harnessing microbes to pioneer environmental biophotoelectrochemistry [J]. | TRENDS IN BIOTECHNOLOGY , 2024 , 42 (12) : 1677-1690 .
MLA Huang, Shaofu et al. "Harnessing microbes to pioneer environmental biophotoelectrochemistry" . | TRENDS IN BIOTECHNOLOGY 42 . 12 (2024) : 1677-1690 .
APA Huang, Shaofu , Ye, Jie , Gao, Jiangtao , Chen, Man , Zhou, Shungui . Harnessing microbes to pioneer environmental biophotoelectrochemistry . | TRENDS IN BIOTECHNOLOGY , 2024 , 42 (12) , 1677-1690 .
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