Zhe-Ming Wang

Pacific Northwest National Laboratory

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John M. Zachara

Pacific Northwest National Laboratory

Kevin M. Rosso

Pacific Northwest National Laboratory

Liang Shi

China University of Geosciences

Chongxuan Liu

Southern University of Science and Technology

Carolyn I. Pearce

Pacific Northwest National Laboratory

ÉW

Éric Walter

Pacific Northwest National Laboratory

Wenwen Cui

Jiangsu Normal University

Bin Yang

Nankai University

Dequan Xiao

University of New Haven

Andrew Lipton

Pacific Northwest National Laboratory

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Pacific Northwest National Laboratory

170

Battelle

Environmental Molecular Sciences Laboratory

Richland College

Washington State University

University of Washington

Physical Sciences (United States)

Office of Scientific and Technical Information

Chinese Academy of Sciences

John Wiley & Sons (United States)

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Rapid electron exchange between surface-exposed bacterial cytochromes and Fe(III) minerals

Proceedings of the National Academy of Sciences (2013)

Gaye F. White Zhi Shi Liang Shi Zhe-Ming Wang Alice Dohnálková

The mineral-respiring bacterium Shewanella oneidensis uses a protein complex, MtrCAB, composed of two decaheme cytochromes, MtrC and MtrA, brought together inside a transmembrane porin, MtrB, to transport electrons across the outer membrane to a variety of mineral-based electron acceptors. A proteoliposome system containing a pool of internalized electron carriers was used to investigate how the topology of the MtrCAB complex relates to its ability to transport electrons across a lipid bilayer to externally located Fe(III) oxides. With MtrA facing the interior and MtrC exposed on the outer surface of the phospholipid bilayer, the established in vivo orientation, electron transfer from the interior electron carrier pool through MtrCAB to solid-phase Fe(III) oxides was demonstrated. The rates were 10 3 times higher than those reported for reduction of goethite, hematite, and lepidocrocite by S. oneidensis , and the order of the reaction rates was consistent with those observed in S. oneidensis cultures. In contrast, established rates for single turnover reactions between purified MtrC and Fe(III) oxides were 10 3 times lower. By providing a continuous flow of electrons, the proteoliposome experiments demonstrate that conduction through MtrCAB directly to Fe(III) oxides is sufficient to support in vivo, anaerobic, solid-phase iron respiration.

Shewanella oneidensis

Lepidocrocite

Ferrihydrite

Electron acceptor

10.1073/pnas.1220074110

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Citations (201)

Continuous, One-pot Synthesis and Post-Synthetic Modification of NanoMOFs Using Droplet Nanoreactors

Scientific Reports (2016)

Sachin Jambovane Satish K. Nune Ryan Kelly B. Peter McGrail Zhe-Ming Wang

Metal-organic frameworks (MOFs); also known as porous coordination polymers (PCP) are a class of porous crystalline materials constructed by connecting metal clusters via organic linkers. The possibility of functionalization leads to virtually infinite MOF designs using generic modular methods. Functionalized MOFs can exhibit interesting physical and chemical properties including accelerated adsorption kinetics and catalysis. Although there are discrete methods to synthesize well-defined nanoscale MOFs, rapid and flexible methods are not available for continuous, one-pot synthesis and post-synthetic modification (functionalization) of MOFs. Here, we show a continuous, scalable nanodroplet-based microfluidic route that not only facilitates the synthesis of MOFs at a nanoscale, but also offers flexibility for direct functionalization with desired functional groups (e.g., -COCH3, fluorescein isothiocyanate; FITC). In addition, the presented route of continuous manufacturing of functionalized nanosized MOFs takes significantly less time compared to state-of-the-art batch methods currently available (1 hr vs. several days). We envisage our approach to be a breakthrough method for synthesizing complex functionalized nanomaterials (metal, metal oxides, quantum dots and MOFs) that are not accessible by direct batch processing and expand the range of a new class of functionalized MOF-based functional nanomaterials.

Surface Modification

Nanoreactor

Nanomaterials

10.1038/srep36657

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Citations (54)

Reductive dissolution of goethite and hematite by reduced flavins

Geochimica et Cosmochimica Acta (2013)

Zhi Shi John M. Zachara Zhe-Ming Wang Liang Shi Jim Fredrickson

Shewanella oneidensis

Ferrihydrite

Reaction rate

10.1016/j.gca.2013.05.039

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Citations (45)

Insights into sorption speciation of uranium on phlogopite: Evidence from TRLFS and DFT calculation

Journal of Hazardous Materials (2021)

Duoqiang Pan Xiaodong Zhao Peng Wang Ping Li Yuhong Li

Phlogopite

Uranyl

10.1016/j.jhazmat.2021.128164

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Citations (14)

Transport of U(VI) through sediments amended with phosphate to induce in situ uranium immobilization

Water Research (2014)

Vrajesh Mehta Fabien Maillot Zhe-Ming Wang Jeffrey G. Catalano Daniel E. Giammar

10.1016/j.watres.2014.11.044

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Citations (48)

Data for EMSL Project 60163 from June 2022

OSTI OAI (U.S. Department of Energy Office of Scientific and Technical Information) (2022)

Zhe-Ming Wang Scott Baker Andrew Lipton Bernd Raschke Jay Bardhan

10.25582/data.2022-06.2530864/2382619

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Surface-Active β-Caryophyllene Oxidation Products at the Air/Aqueous Interface

ACS Earth and Space Chemistry (2019)

Ariana Gray Bé Yangdongling Liu Aashish Tuladhar Aleia D. Bellcross Zhe-Ming Wang

We examine synthesized standards of structurally related β-caryophyllene ozonolysis products at the air/water and air/ammonium sulfate (aq) interfaces using polarization-resolved standard- and high-resolution vibrational sum frequency generation (SFG) spectroscopy in the C–H and O–H stretching regions. β-Caryophyllene aldehyde, the most surface-active molecule in the suite, appears to undergo a change in its molecular orientation distribution when transitioning from low to high relative surface coverage. We also report that the water molecules present at the outermost layer of the aqueous interface are displaced by or hydrogen-bonded to β-caryophyllene aldehyde on both the ammonium sulfate (aq) and water subphases. Additionally, the more weakly hydrogen-bonded water network observed around ∼3400 cm–1 seems to be perturbed to a greater extent by β-caryophyllene aldehyde than the more strongly hydrogen-bonded population observed at ∼3200 cm–1 on the ammonium sulfate (aq) subphase, while this effect is not observed on the water subphase. We provide surface spectroscopic evidence for the "salting out" effect of ammonium sulfate in aqueous environments and discuss the implications for understanding the organization of surface-localized molecules present in aqueous cloud-forming droplets containing dissolved aerosol cloud condensation nuclei (CCN) in the atmosphere. Despite the importance of elucidating the surface activity and interfacial organization of individual molecules in aqueous media, future work will focus on how the combined effects of several surface-active constituents dictate overall cloud activation potentials of aerosol particles.

Interface (matter)

10.1021/acsearthspacechem.9b00185

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Citations (9)

Comparative reactivity study of forsterite and antigorite in wet supercritical CO2 by in situ infrared spectroscopy

International journal of greenhouse gas control (2013)

Christopher J. Thompson John S. Loring Kevin M. Rosso Zhe-Ming Wang

Forsterite

Carbonate minerals

Reactivity

Silicate minerals

Bicarbonate

10.1016/j.ijggc.2013.07.007

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Citations (47)

A trans‐outer membrane porin‐cytochrome protein complex for extracellular electron transfer by G eobacter sulfurreducens PCA

Environmental Microbiology Reports (2014)

Yimo Liu Zhe-Ming Wang Juan Liu Caleb E. Levar Marcus J. Edwards

The multi-heme, outer membrane c-type cytochrome (c-Cyt) OmcB of Geobacter sulfurreducens was previously proposed to mediate electron transfer across the outer membrane. However, the underlying mechanism has remained uncharacterized. In G. sulfurreducens, the omcB gene is part of two tandem four-gene clusters, each is predicted to encode a transcriptional factor (OrfR/OrfS), a porin-like outer membrane protein (OmbB/OmbC), a periplasmic c-type cytochrome (OmaB/OmaC) and an outer membrane c-Cyt (OmcB/OmcC) respectively. Here, we showed that OmbB/OmbC, OmaB/OmaC and OmcB/OmcC of G. sulfurreducens PCA formed the porin-cytochrome (Pcc) protein complexes, which were involved in transferring electrons across the outer membrane. The isolated Pcc protein complexes reconstituted in proteoliposomes transferred electrons from reduced methyl viologen across the lipid bilayer of liposomes to Fe(III)-citrate and ferrihydrite. The pcc clusters were found in all eight sequenced Geobacter and 11 other bacterial genomes from six different phyla, demonstrating a widespread distribution of Pcc protein complexes in phylogenetically diverse bacteria. Deletion of ombB-omaB-omcB-orfS-ombC-omaC-omcC gene clusters had no impact on the growth of G. sulfurreducens PCA with fumarate but diminished the ability of G. sulfurreducens PCA to reduce Fe(III)-citrate and ferrihydrite. Complementation with the ombB-omaB-omcB gene cluster restored the ability of G. sulfurreducens PCA to reduce Fe(III)-citrate and ferrihydrite.

Geobacter sulfurreducens

Porin

ORFS

10.1111/1758-2229.12204

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Citations (177)

Characterization of lignin derived from water-only and dilute acid flowthrough pretreatment of poplar wood at elevated temperatures

Biotechnology for Biofuels (2015)

Libing Zhang Lishi Yan Zhe-Ming Wang Dhrubojyoti D. Laskar Marie Swita

Flowthrough pretreatment of biomass is a critical step in lignin valorization via conversion of lignin derivatives to high-value products, a function vital to the economic efficiency of biorefinery plants. Comprehensive understanding of lignin behaviors and solubilization chemistry in aqueous pretreatment such as water-only and dilute acid flowthrough pretreatment is of fundamental importance to achieve the goal of providing flexible platform for lignin utilization.In this study, the effects of flowthrough pretreatment conditions on lignin separation from poplar wood were reported as well as the characteristics of three sub-sets of lignin produced from the pretreatment, including residual lignin in pretreated solid residues (ReL), recovered insoluble lignin in pretreated liquid (RISL), and recovered soluble lignin in pretreatment liquid (RSL). Both the water-only and 0.05 % (w/w) sulfuric acid pretreatments were performed at temperatures from 160 to 270 °C on poplar wood in a flowthrough reactor system for 2-10 min. Results showed that water-only flowthrough pretreatment primarily removed syringyl (S units). Increased temperature and/or the addition of sulfuric acid enhanced the removal of guaiacyl (G units) compared to water-only pretreatments at lower temperatures, resulting in nearly complete removal of lignin from the biomass. Results also suggested that more RISL was recovered than ReL and RSL in both dilute acid and water-only flowthrough pretreatments at elevated temperatures. NMR spectra of the RISL revealed significant β-O-4 cleavage, α-β deoxygenation to form cinnamyl-like end groups, and slight β-5 repolymerization in both water-only and dilute acid flowthrough pretreatments.Elevated temperature and/or dilute acid greatly enhanced lignin removal to almost 100 % by improving G unit removal besides S unit removal in flowthrough system. Only mild lignin structural modification was caused by flowthrough pretreatment. A lignin transformation pathway was proposed to explain the complexity of the lignin structural changes during hot water and dilute acid flowthrough pretreatment.Graphical abstractLignin transformations in water-only and dilute acid flowthrough pretreatment at elevated temperatures.

10.1186/s13068-015-0377-x

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Citations (96)