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1.
Anal Chem ; 96(4): 1668-1677, 2024 01 30.
Article in English | MEDLINE | ID: mdl-38226847

ABSTRACT

A new matrix framework is presented in this study for the improved ionization efficiency of complex mixtures by matrix-assisted laser desorption ionization (MALDI) mass spectrometry/imaging. Five nitro indole (NI) derivatives [3-methyl-4-nitro-1H-indole (3,4-MNI), 3-methyl-6-nitro-1H-indole (3,6-MNI), 2,3-dimethyl-4-nitro-1H-indole (2,3,4-DMNI), 2,3-dimethyl-6-nitro-1H-indole (2,3,6-DMNI), and 4-nitro-1H-indole (4-NI)] were synthesized and shown to produce both positive and negative ions with a broad class of analytes as MALDI matrices. NI matrices were compared to several common matrices, such as 2,5-dihydroxybenzoic acid (DHB), alpha-cyano-4-hydroxylcinnamic acid (CHCA), sinapinic acid (SA), 1,5-diaminonaphthelene (1,5-DAN), and 9-aminoacridine (9-AA), for the analysis of lipid, peptide, protein, glycan, and perfluorooctanesulfonic acid (PFOS) compounds. 3,4-MNI demonstrated the best performance among the NI matrices. This matrix resulted in reduced ion suppression and better detection sensitivity for complex mixtures, for example, egg lipids/milk proteins/PFOS in tap water, while 2,3,6-DMNI was the best matrix for blueberry tissue imaging. Several important aspects of this work are reported: (1) dual-polarity ion production with NI matrices and complex mixtures; (2) quantitative analysis of PFOS with a LOQ of 0.5 ppb in tap water and 0.05 ppb in MQ water (without solid phase extraction enrichment), with accuracy and precision within 5%; (3) MALDI imaging with 2,3,6-DMNI as a matrix for plant metabolite/lipid identification with ionization enhancement in the negative ion mode m/z 600-900 region; and (4) development of a thin film deposition under/above tissue method for MALDI imaging with a vacuum sublimation matrix on a high-vacuum MALDI instrument.


Subject(s)
Alkanesulfonic Acids , Fluorocarbons , Indoles , Lipids , Spectrometry, Mass, Matrix-Assisted Laser Desorption-Ionization/methods , Lipids/analysis , Complex Mixtures , Water
2.
Sci Total Environ ; 876: 162703, 2023 Jun 10.
Article in English | MEDLINE | ID: mdl-36906032

ABSTRACT

Dissolved organic matter (DOM) in the sediment matrix affects contaminant remediation through consumption of oxidants and binding with contaminants. Yet the change in DOM during remediation processes, particularly during electrokinetic remediation (EKR), remains under-investigated. In this work, we elucidated the fate of sediment DOM in EKR using multiple spectroscopic tools under abiotic and biotic conditions. We found that EKR led to significant electromigration of the alkaline-extractable DOM (AEOM) toward the anode, followed by transformation of the aromatics and mineralization of the polysaccharides. The AEOM remaining in the cathode (largely polysaccharides) was resistant to reductive transformation. Limited difference was noted between abiotic and biotic conditions, indicating the dominance of electrochemical processes when relatively high voltages were applied (1-2 V/cm). The water-extractable organic matter (WEOM), in contrast, showed an increase at both electrodes, which was likely attributable to pH-driven dissociations of humic substances and amino acid-type constituents at the cathode and the anode, respectively. Nitrogen migrated with the AEOM toward the anode, but phosphorus remained immobilized. Understanding the redistribution and transformation of DOM could inform studies on contaminant degradation, carbon and nutrient availability, and sediment structural changes in EKR.

3.
Nat Commun ; 13(1): 5758, 2022 Sep 30.
Article in English | MEDLINE | ID: mdl-36180443

ABSTRACT

Population and development megatrends will drive growth in cement production, which is already one of the most challenging-to-mitigate sources of CO2 emissions. However, availabilities of conventional secondary cementitious materials (CMs) like fly ash are declining. Here, we present detailed generation rates of secondary CMs worldwide between 2002 and 2018, showing the potential for 3.5 Gt to be generated in 2018. Maximal substitution of Portland cement clinker with these materials could have avoided up to 1.3 Gt CO2-eq. emissions (~44% of cement production and ~2.8% of anthropogenic CO2-eq. emissions) in 2018. We also show that nearly all of the highest cement producing nations can locally generate and use secondary CMs to substitute up to 50% domestic Portland cement clinker, with many countries able to potentially substitute 100% Portland cement clinker. Our results highlight the importance of pursuing regionally optimized CM mix designs and systemic approaches to decarbonizing the global CMs cycle.

4.
Proc Natl Acad Sci U S A ; 119(18): e2105006119, 2022 05 03.
Article in English | MEDLINE | ID: mdl-35467985

ABSTRACT

The world has committed trillions in fiscal expenditures to reboot the economy in the post­COVID-19 era. However, the effectiveness and the equity impacts of current fiscal stimuli are not fully understood. Using an extended adaptive regional input­output model, we assess the short-term impacts (2020 through 2022) of feasible stimuli on the global economy and the labor market. Our findings show that the stimuli pledged by 26 countries, i.e., 2.4 trillion euros in total, are effective in keeping the recession short and shallow by saving 53 million to 57 million jobs (compared to the no-stimulus scenario). However, the stimuli exacerbate income inequity at the global scale if we define "equity" as those who suffer more from the pandemic should receive more assistance. Low-skilled workers in these countries, who suffer more from the pandemic than high-skilled workers, benefit 38 to 41% less from the job-creation effects of the current fiscal stimuli. As an alternative, low-carbon stimuli can achieve a balance between effectiveness and equity at the global level. Low-carbon stimuli save 55 million to 58 million jobs and decrease income inequality by 2 to 3% globally compared to the currently pledged stimuli. Country-level situations are more complicated, as modifying the current stimuli to achieve more "greenness" brings win­win in effectiveness and equity in some countries, while in the others, more greenness and equity are at the expense of less job savings. Our findings underscore the need to consider the overlooked trade-offs between effectiveness, equity, and greenness, both globally and nationally, when designing further postpandemic fiscal stimuli.


Subject(s)
Employment , Income , Climate Change , Humans
5.
Water Res ; 205: 117677, 2021 Oct 15.
Article in English | MEDLINE | ID: mdl-34624586

ABSTRACT

Previous laboratory scale studies indicate nanofiltration (NF) and UV-sulfite photochemical treatments as promising technologies for the removal and destruction, respectively, of per- and polyfluoroalkyl substances (PFASs) from contaminated water. This study reports on a field demonstration of a pilot-scale hybrid NF and UV-sulfite treatment train for the remediation of 12 PFASs detected in groundwater impacted by aqueous film-forming foam (AFFF) at a U.S. Department of Defense installation. For most of the detected PFASs, NF rejection was consistently ≥ 95% over a 30-day field trial when operating at 90% total permeate recovery. Rejection of short-chain perfluorosulfonic acids (PFSAs) by NF decreased when recoveries increased from 90 to 97%; tests with a reverse osmosis (RO) membrane showed ≥ 99% rejection of all PFASs regardless of increasing recovery. UV treatment of the NF reject following 90% permeate recovery resulted in variable destruction of individual PFASs, with rates also being dependent on pH and the identity and concentration of UV photosensitizer. Rates of perfluorocarboxylic acid (PFCA) degradation were greater than those measured for PFSAs and perfluoroalkyl acid (PFAA) precursors and were independent of perfluoroalkyl chain length. In contrast, rates of PFSA degradation increased with increasing chain length. Consistent levels of PFAS degradation by UV-sulfite were observed during a 30-day demonstration experiment in NF reject water amended with 10 mM sulfite and adjusted to pH 11.2. Collectively, > 75% of the detected PFAS mass in the NF reject was destroyed after 4 h of UV treatment, increasing to > 90% after 8 h of treatment. An analysis of electrical energy inputs for the hybrid NF/UV-sulfite treatment train showed energy per order magnitude (EE/O) requirements ranging from ≤ 13.1 kWh/m3 for PFCAs and 14.1 kWh/m3 for PFOS to values > 100 kWh/m3 for more recalcitrant short-chain PFSA analogues. The UV reactor and water-cooling system were the major contributors to overall energy requirements and represent the greatest opportunities for improving efficiency of the technology.


Subject(s)
Fluorocarbons , Groundwater , Water Pollutants, Chemical , Fluorocarbons/analysis , Sulfites , Water , Water Pollutants, Chemical/analysis
6.
Waste Manag ; 118: 563-572, 2020 Dec.
Article in English | MEDLINE | ID: mdl-32987347

ABSTRACT

Non-hazardous industrial waste (NHIW), primarily consisting of manufacturing process residues, has long been overlooked in waste reporting, regulation, and reuse. Limited information about NHIW generation with spatial and sectoral details has impeded the systematization of reuse efforts to move towards a resource-efficient economy. In this article, we develop a methodological framework that makes the best use of fragmented and limited observational data to infer the confidence intervals of NHIW generation by sector, location, and year across the United States. The framework decomposes the quantity of NHIW into two factors: the activity level (economic output) and the waste intensity factor (waste tonnage generated per unit of output). It statistically infers the probability distribution of the waste intensity factor and extrapolates waste tonnages to the entire country. In our demonstrative application of the method, we provide an updated estimate for spent foundry sand and find that its total amount in the United States decreased from 2.2-7.1 million tons in 2004 to 1.4-4.7 million tons in 2014. The spatial distribution, however, was highly uneven, with over 90% of the waste generated in 10% of the counties, indicating great variations in reuse potentials and benefits among regions. Our methodological framework makes a significant departure from existing estimations that usually rely on averaging limited observations or expert judgments biased by subjectivity. Detailing spatial and sectoral distributions and temporal trends in NHIW generation and reuse benefits, our study could inform more systematic strategies on waste and materials management to build a circular economy.


Subject(s)
Hazardous Waste , Waste Management , Industrial Waste , Industry , Sand , United States
7.
Water Res ; 184: 116214, 2020 Oct 01.
Article in English | MEDLINE | ID: mdl-32726737

ABSTRACT

Anaerobic digestion (AD) is one of the most widely adopted bioenergy recovery technologies globally. Despite the wide adoption, AD has been challenged by the unstable performances caused by imbalanced substrate and/or electron availability among different reaction steps. Bioelectrochemical anaerobic digestion (BEAD) is a promising concept that has demonstrated potential for balancing the electron transfer rates and enhancing the methane yield in AD during shocks. While great progress has been made, a wide range of, and sometimes inconsistent engineering and technical strategies were attempted to improve BEAD. To consolidate past efforts and guide future development, a comprehensive review of the fundamental bioprocesses in BEAD is provided herein, followed by a critical evaluation of the engineering and technical optimizations attempted thus far. Further, a few novel directions and strategies that can enhance the performance and practicality of BEAD are proposed for future research to consider. This review and outlook aim to provide a fundamental understanding of BEAD and inspire new research ideas in AD and BEAD in a mechanism-informed fashion.


Subject(s)
Bioreactors , Methane , Anaerobiosis , Electrodes , Electron Transport
8.
Environ Sci Technol ; 54(12): 7651-7658, 2020 06 16.
Article in English | MEDLINE | ID: mdl-32469515

ABSTRACT

Living Filtration Membranes (LFMs) are a water filtration technology that was recently developed in the lab (Technology Readiness Level 4). LFMs have shown filtration performance comparable with that of ultrafiltration, far better fouling resistance than conventional polymer membranes, and good healing capabilities. These properties give LFMs promise to address two significant issues in conventional membrane filtration: fouling and membrane damage. To integrate environmental considerations into future technology development (i.e., Ecodesign), this study assesses the life cycle environmental performance of drinking water treatment using LFMs under likely design and operation conditions. It also quantitatively ranks the engineering design and operation factors governing the further optimization of LFM environmental performance using a global sensitivity analysis. The results suggest that LFMs' superior fouling resistance will reduce the life cycle environmental impacts of ultrafiltration by 25% compared to those of a conventional polymer membrane in most impact categories (e.g., acidification, global warming potential, and carcinogenics). The only exception is the eutrophication impact, where the need for growth medium and membrane regeneration offsets the benefits of LFMs' fouling resistance. Permeability is the most important factor that should be prioritized in future R&D to further improve the life cycle environmental performance of LFMs. A 1% improvement in the permeability will lead to a ∼0.7% improvement in LFMs' environmental performance in all the impact categories, whereas the same change in the other parameters investigated (e.g., LFM lifespan and regeneration frequency) typically only leads to a <0.2% improvement.


Subject(s)
Membranes, Artificial , Water Purification , Filtration , Permeability , Ultrafiltration
9.
Environ Sci Technol ; 54(11): 6908-6918, 2020 06 02.
Article in English | MEDLINE | ID: mdl-32352763

ABSTRACT

In this study, we present a holistic analysis of the stock and emissions of poly- and perfluoroalkyl substances (PFAS) in California carpet in 2000-2030. Our high estimate is that, in 2017, the total PFAS accumulated in in-use carpet stock and landfilled carpet are ∼60 and ∼120 tonnes, respectively, and the resultant PFAS emissions are ∼800 and ∼100 kg, respectively. Among the three subclasses (side-chain polymers, PFAA, and nonpolymeric precursors), side-chain polymers dominate the in-use stock and landfill accumulation, while nonpolymeric precursors dominate the resultant emissions. Our low estimate is typically 8-15% of the high estimate and follows similar trends and subclass breakdowns as the high estimate. California's new Carpet Stewardship Regulations (24% recycling of end-of-life carpet) will reduce the landfilled PFAS by 6% (7 tonnes) at the cost of increasing the in-use stock by 2% (2 tonnes) in 2030. Aggressive PFAS phase-out by carpet manufacturers (i.e., reduce PFAS use by 15% annually starting 2020) could reduce the in-use PFAS stock by 50% by 2030, but its impact on the total landfilled PFAS is limited. The shift toward short-chain PFAS will also significantly reduce the in-use stock of long-chain PFAS in carpet by 2030 (only 25% of the total PFAS will be long-chain). Among the data gaps identified, a key one is the current area-based PFAS emission reporting (i.e., g PFAS emitted/area carpet/time), which leads to the counterintuitive result that reducing the PFAS use in carpet production has no impact on the PFAS emissions from in-use stock and landfills. Future technical studies should either confirm this or consider a mass-based unit (e.g., g PFAS emitted/g PFAS used/time) for better integration into regional substance flow analysis. Other noticeable data gaps include the lack of time-series data on emissions from the in-use stock and on leaching of side-chain polymers from landfills.


Subject(s)
Fluorocarbons , Water Pollutants, Chemical , California , Floors and Floorcoverings , Fluorocarbons/analysis , Waste Disposal Facilities , Water Pollutants, Chemical/analysis
10.
Sci Total Environ ; 713: 136698, 2020 Apr 15.
Article in English | MEDLINE | ID: mdl-32019036

ABSTRACT

Bio-electrochemical denitrification (BED) is a promising organic carbon-free nitrate remediation technology. However, the relationship between engineering conditions, biofilm community composition, and resultant functions in BED remains under-explored. This study used deep sequencing and variation partitioning analysis to investigate the compositional shifts in biofilm communities under varied poised potentials in the batch mode, and correlated these shifts to reactor-level functional differences. Interestingly, the results suggest that the proliferation of a key species, Thiobacillus denitrificans, and community diversity (the Shannon index), were almost equally important in explaining the reactor-to-reactor functional variability (e.g. variability in denitrification rates was 51% and 38% attributable to key species and community diversity respectively, with a 30% overlap), but neither was heavily impacted by the poised potential. The findings suggest that while enriching the key species may be critical in improving the functional efficiency of BED, poised potentials may not be an effective strategy to achieve the desired level of enrichment in substrate-limited real-world conditions.


Subject(s)
Denitrification , Biofilms , Bioreactors , Nitrates , Thiobacillus
11.
Sci Total Environ ; 706: 135684, 2020 Mar 01.
Article in English | MEDLINE | ID: mdl-31862588

ABSTRACT

The recent discovery of complete ammonia oxidation (comammox) process in a single organism challenged the division of labor between two functional groups in the classical two-step nitrification model. However, the distribution and activity of comammox bacteria in various environments remain largely unknown. This study presented a large-scale investigation of the geographical distribution, phylogenetic diversity, and activity of comammox Nitrospira in typical agricultural soils. Among the 23 samples harvested across China, comammox Nitrospira clade A was ubiquitously detected at 4.14 × 104-1.65 × 107amoA gene copies/g dry soil, with 90% belonging to the subclade A2. The abundance of comammox Nitrospira clade B was two orders of magnitude lower than clade A. In all samples, comammox Nitrospira were 1-2 orders of magnitude less abundant than canonical nitrifiers, and soils with slightly high pH and C/N tended to enrich more comammox Nitrospira. Unlike canonical nitrifiers, comammox Nitrospira had sustained amoA gene transcription regardless of external ammonia supply, indicating their competitive advantage over other nitrifiers under low-ammonia conditions. When fed with 1 mM ammonium for 15 days, comammox Nitrospira in tested soils were enriched 2.36 times higher than those enriched by the same amount of nitrite, indicating their preference to utilizing ammonia as the substrate. DNA-SIP further confirmed the in situ nitrification activity of comammox Nitrospira. This study provided new insights into the broad distribution and diversity of comammox Nitrospira in agricultural soils, which could potentially play an important role in the microbial nitrogen cycle in soils.


Subject(s)
Nitrification , Soil , Ammonia , Archaea , Bacteria , China , Oxidation-Reduction , Phylogeny , Soil Microbiology
12.
Environ Sci Technol ; 52(6): 3706-3715, 2018 03 20.
Article in English | MEDLINE | ID: mdl-29436224

ABSTRACT

Bisphenol A (BPA), a synthetic organic chemical, is creating a new category of ecological and human health challenges due to unintended leakage. Effectively managing the use and leakage of BPA can benefit from an understanding of the anthropogenic BPA cycles (i.e., the size of BPA flows and stocks). In this work, we provide a dynamic analysis of the anthropogenic BPA cycles in China for 2000-2014. We find that China's BPA consumption has increased 10-fold since 2000, to ∼3 million tonnes/year. With the increasing consumption, China's in-use BPA stock has increased 500-fold to 14.0 million tonnes (i.e., 10.2 kg BPA/capita). It is unclear whether a saturation point has been reached, but in 2004-2014, China's in-use BPA stock has been increasing by 0.8 kg BPA/capita annually. Electronic products are the biggest contributor, responsible for roughly one-third of China's in-use BPA stock. Optical media (DVD/VCD/CDs) is the largest contributor to China's current End-of-Life (EoL) BPA flow, totaling 0.9 million tonnes/year. However, the EoL BPA flow due to e-waste will increase quickly, and will soon become the largest EoL BPA flow. The changing quantities and sources of EoL BPA flows may require a shift in the macroscopic BPA management strategies.


Subject(s)
Benzhydryl Compounds , Phenols , China , Humans
13.
Environ Sci Technol ; 51(15): 8654-8662, 2017 Aug 01.
Article in English | MEDLINE | ID: mdl-28616965

ABSTRACT

Bisphenol A (BPA), a widely used petrochemical compound, has become an emerging global environmental management challenge because its leakage is associated with potential environmental and human health impacts. Until now, available BPA statistics have been limited to the products that directly use BPA. In this study, we delineate direct and indirect BPA flows for the 2012 Chinese economy. We find that construction, production of educational and recreational products, and automobile manufacturing are the most BPA-intensive sectors in terms of total BPA flows (300, 157, and 130 Gg total BPA flows, respectively). The public management and health sectors, however, incur significant indirect BPA flows, defined as embedded and inter-sectoral BPA placed into use, even though direct BPA use by these sectors is limited. By revealing the currently overlooked indirect BPA flows, this study reveals data gaps that are highly relevant to improving the accuracy of estimated BPA flows and losses. The method used herein is transferrable to other emerging and environmentally relevant materials, thereby providing the holistic understanding needed for cities, regions, or nations to design effective policy interventions.


Subject(s)
Benzhydryl Compounds/economics , Commerce , Phenols/economics , China , Cities , Environment , Humans
14.
J Hazard Mater ; 338: 296-305, 2017 Sep 15.
Article in English | MEDLINE | ID: mdl-28578231

ABSTRACT

In this study, Fe-Mn binary oxides, which harbor the strong oxidative power of manganese dioxide and the high adsorption capacity of iron oxides, were synthesized for Tl(I) removal using a concurrent chemical oxidation and precipitation method. The adsorption of Tl onto the Fe-Mn adsorbent was fast, effective, and selective, with equilibrium sorption reaching over 95% under a broad operating pH (3-12), and high ionic strength (0.1-0.5mol/L). The adsorption can be well fitted with both Langmuir and Freundlich isotherms, and the kinetics can be well described by the pseudo-second-order model. Fourier transform infrared (FT-IR) and X-ray photoelectron spectroscopy (XPS) spectra suggest that surface complexation, oxidation and precipitation were the main mechanisms for the removal of Tl. This study shows that the Fe-Mn binary oxides could be a promising adsorbent for Tl removal.

15.
J Hazard Mater ; 333: 179-185, 2017 Jul 05.
Article in English | MEDLINE | ID: mdl-28355586

ABSTRACT

Simultaneous removal of thallium (Tl) and chloride from a highly saline industrial wastewater was investigated using modified anion ion exchange resins. The removal of thallium was mainly driven by the exchange of Tl-chlorocomplex (TlCl4-) formed in the oxidation of thallous (Tl (I)) to thallic ion (Tl (III)) by hydrogen peroxide (H2O2) under saline conditions. Over 97% of thallium and chloride removal was achieved using the modified resins, with a wide optimal conditions found to be H2O2 dosage 1.0-25.0mL/L, pH 1.6-4.3, and flow rate 0.5-4.7mL/L. The modified resins had an exchange capacity of 4.771mg Tl/g dry resins for thallium and 1800mg Cl/g dry resins for chloride. Stable regeneration could be achieved with the modified resins: over 97% of thallium and 90% of chloride can be eluted using Na2SO3 solution and alternating hot (60°C) H2SO4 and cold (25°C) water, and over 98% removal of thallium and chloride was achieved after five consecutive regeneration cycles.

16.
Environ Sci Technol ; 51(1): 320-327, 2017 01 03.
Article in English | MEDLINE | ID: mdl-27943673

ABSTRACT

Municipal solid waste (MSW) disposal represents one of the largest sources of anthropogenic greenhouse gas (GHG) emissions. However, the biogenic GHG emissions in the predisposal stage of MSW management (i.e., the time from waste being dropped off in community or household garbage bins to being transported to disposal sites) are excluded from the IPCC inventory methodology and rarely discussed in academic literature. Herein, we quantify the effluxes of carbon dioxide (CO2), methane (CH4), and nitrous oxide (N2O) from garbage bins in five communities along the urban-rural gradient in Beijing in four seasons. We find that the annual average CO2, CH4, and N2O effluxes in the predisposal stage were (1.6 ± 0.9)103, 0.049 ± 0.016, and 0.94 ± 0.54 mg kg-1h-1 (dry matter basis) and had significant seasonal differences (24- to 159-fold) that were strongly correlated with temperature. According to our estimate, the N2O emission in the MSW predisposal stage amounts to 20% of that in the disposal stage in Beijing, making the predisposal stage a nontrivial source of waste-induced N2O emissions. Furthermore, the CO2 and CH4 emissions in the MSW predisposal account for 5% (maximum 10% in summer) of the total carbon contents in a Beijing's household food waste stream, which has significance in the assessment of MSW-related renewable energy potential and urban carbon cycles.


Subject(s)
Greenhouse Effect , Solid Waste , Carbon Dioxide , Methane , Nitrous Oxide , Refuse Disposal , Waste Management
17.
Bioresour Technol ; 215: 380-385, 2016 Sep.
Article in English | MEDLINE | ID: mdl-27020397

ABSTRACT

This study reports that wastewater can be used to capture and store CO2 directly from ambient air and produce energy. The proof-of-concept system consisted of an ion exchange resin column that captures and concentrates ambient CO2 using a moisture-driven cycle. The concentrated CO2 was then transferred into a microbial electrochemical carbon capture (MECC) reactor for carbon sequestration and hydrogen production. Data from an average batch cycle showed that approximately 8mmol/L CO2 was captured in the MECC cathode when 0.14g/LCOD was removed in the anode. With 90% hydrogen conversion efficiency, the energy intensity and CO2 absorption from the process could be 11.3kJ/gCOD and 0.49gCO2/gCOD respectively. If the proposed process is applied, over 68milliontons of atmospheric CO2 can be captured yearly during wastewater treatment in the US, which equates to significant economic values if CO2 taxes were to be implemented more widely.


Subject(s)
Carbon Sequestration , Electrolysis/methods , Waste Management/methods , Wastewater/chemistry , Carbon/metabolism , Carbon Dioxide/isolation & purification , Carbon Dioxide/metabolism , Electrochemical Techniques/methods , Electrodes , Humans , Hydrogen/metabolism
18.
PLoS One ; 9(1): e85575, 2014.
Article in English | MEDLINE | ID: mdl-24475045

ABSTRACT

Soil biogeochemical processes and the ecological stability of wetland ecosystems under global warming scenarios have gained increasing attention worldwide. Changes in the capacity of microorganisms to maintain stoichiometric homeostasis, or relatively stable internal concentrations of elements, may serve as an indicator of alterations to soil biogeochemical processes and their associated ecological feedbacks. In this study, an outdoor computerized microcosm was set up to simulate a warmed (+5°C) climate scenario, using novel, minute-scale temperature manipulation technology. The principle of stoichiometric homeostasis was adopted to illustrate phosphorus (P) biogeochemical cycling coupled with carbon (C) dynamics within the soil-microorganism complex. We hypothesized that enhancing the flux of P from soil to water under warming scenarios is tightly coupled with a decrease in homeostatic regulation ability in wetland ecosystems. Results indicate that experimental warming impaired the ability of stoichiometric homeostasis (H) to regulate biogeochemical processes, enhancing the ecological role of wetland soil as an ecological source for both P and C. The potential P flux from soil to water ranged from 0.11 to 34.51 mg m(-2) d(-1) in the control and 0.07 to 61.26 mg m(-2) d(-1) in the warmed treatment. The synergistic function of C-P acquisition is an important mechanism underlying C∶P stoichiometric balance for soil microorganisms under warming. For both treatment groups, strongly significant (p<0.001) relationships fitting a negative allometric power model with a fractional exponent were found between n-HC∶P (the specialized homeostatic regulation ability as a ratio of soil highly labile organic carbon to dissolved reactive phosphorus in porewater) and potential P flux. Although many factors may affect soil P dynamics, the n-HC∶P term fundamentally reflects the stoichiometric balance or interactions between the energy landscape (i.e., C) and flow of resources (e.g., N and P), and can be a useful ecological tool for assessing potential P flux in ecosystems.


Subject(s)
Homeostasis/physiology , Models, Biological , Phosphorus/metabolism , Soil Microbiology , Soil/chemistry , Temperature , Wetlands , Ecological and Environmental Phenomena , Global Warming
19.
PLoS One ; 8(5): e61141, 2013.
Article in English | MEDLINE | ID: mdl-23667435

ABSTRACT

Agricultural fertilization may change processes of elemental biogeochemical cycles and alter the ecological function. Ecoenzymatic stoichiometric feature plays a critical role in global soil carbon (C) metabolism, driving element cycles, and mediating atmospheric composition in response to agricultural nutrient management. Despite the importance on crop growth, the role of phosphorous (P) in compliance with eco-stoichiometry on soil C and nitrogen (N) sequestration in the paddy field remains poorly understood in the context of climate change. Here, we collected soil samples from a field experiment after 6 years of chemical P application at a gradient of 0 (P-0), 30 (P-30), 60 (P-60), and 90 (P-90) kg ha(-1) in order to evaluate the role of P on stoichiometric properties in terms of soil chemical, microbial biomass, and eco-enzyme activities as well as greenhouse gas (GHG: CO2, N2O and CH4) emissions. Continuous P input increased soil total organic C and N by 1.3-9.2% and 3%-13%, respectively. P input induced C and N limitations as indicated by the decreased ratio of C:P and N:P in the soil and microbial biomass. A synergistic mechanism among the ecoenzymatic stoichiometry, which regulated the ecological function of microbial C and N acquisition and were stoichiometrically related to P input, stimulated soil C and N sequestration in the paddy field. The lower emissions of N2O and CH4 under the higher P application (P-60 and P-90) in July and the insignificant difference in N2O emission in August compared to P-30; however, continuous P input enhanced CO2 fluxes for both samplings. There is a technical conflict for simultaneously regulating three types of GHGs in terms of the eco-stoichiometry mechanism under P fertilization. Thus, it is recommended that the P input in paddy fields not exceed 60 kg ha(-1) may maximize soil C sequestration, minimize P export, and guarantee grain yields.


Subject(s)
Agriculture , Ecosystem , Fertilizers/analysis , Phosphorus/pharmacology , Soil/chemistry , Biomass , Gases/chemistry , Greenhouse Effect , Soil Microbiology
20.
Appl Biochem Biotechnol ; 160(1): 182-96, 2010 Jan.
Article in English | MEDLINE | ID: mdl-19214793

ABSTRACT

Microbial fuel cell (MFC) is an emerging biotechnology to convert the organic substrates in wastewater to electricity by anaerobic electrogenic bacteria. The main challenge for MFC research is to elucidate the fundamental mechanisms of electron generation and transfer and to apply these mechanisms to improve the power production in the engineering operation. This study extensively investigated the effects of three inocula (Geobacter sulfurreducens, soil, and wastewater) on the power production and electrochemical characteristics (i.e., internal resistances, Coulombic Efficiency) of MFCs. The results showed that the extents of bacterial adhesion varied between mixed cultures (soil) and pure cultures (G. sulfurreducens). The voltage output increased 30% when bacterial adhesion was well-developed in the soil inocula. Meanwhile, the inoculum types clearly affected the internal resistance (R(in)) and power production of MFCs. Pure culture inoculum (G. sulfurreducens) had the lowest R(in) (165 Omega) and the highest Coulombic Efficiency (CE, 25.8%) and Energy Conversion Efficiency (ECE, 7.2%), while the mixed culture inocula (soil) with the high concentration of nonelectrogenic bacteria, exhibited the highest R(in) (620 Omega), lowest CE (9.2%) and lowest ECE (2.4%). Additionally, a second-order correlation was established between the anode potential (P(A)) and power output while an exponential correlation was established between the difference between anode and cathode potentials (DeltaP(C-A)) and power output.


Subject(s)
Bacterial Adhesion , Bioelectric Energy Sources/microbiology , Geobacter/growth & development , Electric Impedance , Electrochemistry , Electrodes , Geobacter/physiology , Oxidation-Reduction , Soil , Solutions , Suspensions
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