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Li, Jun

Publications and source records attributed to Li, Jun.

At least 163 records · Page 9

Genomics insights into ecotype formation of ammonia‐oxidizing archaea in the deep ocean

Summary Various lineages of ammonia‐oxidizing archaea (AOA) are present in deep waters, but the mechanisms that determine ecotype formation are obscure. We studied 18 high‐quality genomes of the marine group I AOA lineages (alpha, gamma and delta) from the Mariana and Ogasawara trenches. The genomes of alpha AOA resembled each other, while those of gamma and delta lineages were more divergent and had even undergone insertion of some phage genes. The instability of the gamma and delta AOA genomes could be partially due to the loss of DNA polymerase B ( polB) and methyladenine DNA glycosylase ( tag ) genes responsible for the repair of point mutations. The alpha AOA genomes harbour genes encoding a thrombospondin‐like outer membrane structure that probably serves as a barrier to gene flow. Moreover, the gamma and alpha AOA lineages rely on vitamin B 12 ‐independent MetE and B 12 ‐dependent MetH, respectively, for methionine synthesis. The delta AOA genome contains genes involved in uptake of sugar and peptide perhaps for heterotrophic lifestyle. Our study provides insights into co‐occurrence of cladogenesis and anagenesis in the formation of AOA ecotypes that perform differently in nitrogen and carbon cycling in dark oceans.

Wang, Yong↗

Wrinkled Graphene Cages as Hosts for High-Capacity Li Metal Anodes Shown by Cryogenic Electron Microscopy

Lithium (Li) metal has long been considered the “holy grail” of battery anode chemistry but is plagued by low efficiency and poor safety due to its high chemical reactivity and large volume fluctuation, respectively. Here we introduce a new host of wrinkled graphene cage (WGC) for Li metal. Different from recently reported amorphous carbon spheres, WGC show highly improved mechanical stability, better Li ion conductivity, and excellent solid electrolyte interphase (SEI) for continuous robust Li metal protection. At low areal capacities, Li metal is preferentially deposited inside the graphene cage. Cryogenic electron microscopy characterization shows that a uniform and stable SEI forms on the WGC surface that can shield the Li metal from direct exposure to electrolyte. With increased areal capacities, Li metal is plated densely and homogeneously into the outer pore spaces between graphene cages with no dendrite growth or volume change. As a result, a high Coulombic efficiency (CE) of ~98.0% was achieved under 0.5 mA/cm 2 and 1–10 mAh/cm 2 in commercial carbonate electrolytes, and a CE of 99.1% was realized with high-concentration electrolytes under 0.5 mA/cm 2 and 3 mAh/cm 2 . Full cells using WGC electrodes with prestored Li paired with Li iron phosphate showed greatly improved cycle lifetime. With 10 mAh/cm 2 Li metal deposition, the WGC/Li composite anode was able to provide a high specific capacity of ~2785 mAh/g. Furthermore, with its roll-to-roll compatible fabrication procedure, WGC serves as a highly promising material for the practical realization of Li metal anodes in next-generation high energy density secondary batteries.

36 MATERIALS SCIENCE↗

Ionization injection of highly-charged copper ions for laser driven acceleration from ultra-thin foils

Laser-driven ion acceleration is often analyzed assuming that ionization reaches a steady state early in the interaction of the laser pulse with the target. This assumption breaks down for materials of high atomic number for which the ionization occurs concurrently with the acceleration process. Using particle-in-cell simulations, we have examined acceleration and simultaneous field ionization of copper ions in ultra-thin targets (20-150 nm thick) irradiated by a laser pulse with intensity 1 × 10 21 W/cm 2 . At this intensity, the laser pulse drives strong electric fields at the rear side of the target that can ionize Cu to charge states with valence L-shell or full K-shell. The highly-charged ions are produced only in a very localized region due to a significant gap between the M- and L-shells' ionization potentials and can be accelerated by strong, forward-directed sections of the field. Such an "ionization injection" leads to well-pronounced bunches of energetic, highly-charged ions. We also find that for the thinnest target (20 nm) a push by the laser further increases the ion energy gain. Thus, the field ionization, concurrent with the acceleration, offers a promising mechanism for the production of energetic, high-charge ion bunches.

43 PARTICLE ACCELERATORS↗

Polarization-based plug-and-play measurement-device-independent quantum key distribution

Measurement-device-independent quantum key distribution (MDI-QKD) has received much attention, with the goal of overcoming all of the security loopholes caused by an imperfect detection system. We here propose a plug-and-play MDI-QKD (P&P MDI-QKD) scheme whereby an untrusted relay node, Charlie, owns a laser and sends photons to Alice and Bob. Alice (Bob) modulates the polarization of the incident photons and returns them to Charlie. Charlie uses a modified Bell state analyzer (BSA) to perform Bell state measurements (BSM). In comparison with the original version of MDI-QKD, our scheme exploits a single untrusted laser as the photon source. This makes the signal photons identical and enhances the Hong-Ou-Mandel effect. Second, because of the P&P structure, the setup can automatically eliminate the birefringence influence of the fibers, which makes the setup highly stable. Finally, our modified BSA can identify |Φ〉{sup +} and |Φ〉{sup −} of four Bell states with polarization encoding but not |Ψ〉{sup +} and |Ψ〉{sup −}. Based on practical experimental parameters, a simulation showed that the maximum theoretical secure transmission distance could reach more 280 km.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Heteroatom-Doped Porous Carbon Materials with Unprecedented High Volumetric Capacitive Performance

The design of carbon-based materials with a high mass density and large porosity has always been a challenging goal, since they fulfill the demands of next-generation supercapacitors and other electrochemical devices. We report a new class of high-density heteroatom-doped porous carbon that can be used as an aqueous-based supercapacitor material. The material was synthesized by an in situ dehalogenation reaction between a halogenated conjugated diene and nitrogen-containing nucleophiles. Under the given conditions, pyridinium salts can only continue to perform the dehalogenation if there is residue water remaining from the starting materials. The obtained carbon materials are highly doped by various heteroatoms, leading to high densities, abundant multimodal pores, and an excellent volumetric capacitive performance. Porous carbon tri-doped with nitrogen, phosphorous, and oxygen exhibits a high packing density (2.13 g cm -3 ) and an exceptional volumetric energy density (36.8 Wh L -1 ) in alkaline electrolytes, making it competitive to even some Ni-MH cells.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Discharge Permit DP-1845 Quarterly Report (July — September 2018)

Discharge Permit (DP)-1845 was issued by the New Mexico Environment (NMED) Ground Water Quality Bureau (GWQB) for discharges via up to three injection wells in a phased Treatability Study of in-situ bioremediation of groundwater at the Sandia National Laboratories, New Mexico, Technical Area-V Groundwater Area of Concern. This report fulfills the quarterly reporting requirements set forth in DP-1845, Section IV.B, Monitoring and Reporting. This reporting period is July 1 through September 30, 2018. The report is due to NMED GWQB by February 1, 2019.

54 ENVIRONMENTAL SCIENCES↗

Effect of processing conditions on additive DISC patterning of P3HT films

There is a critical need to develop a method to pattern semiconducting polymers for device applications on the sub-micrometer scale. Dopant induced solubility control (DISC) patterning is a recently published method for patterning semiconductor polymers that has demonstrated sub-micron resolution. DISC relies on the sequential addition of molecular dopants (here 2,3,5,6-tetrafluoro-7,7,8,8-tetracyanoquinodimethane (F4TCNQ)) to the conjugated polymer. In doped areas, the conjugated polymer is protected from dissolution while in undoped areas, the polymer dissolves into solution. Here we examine factors that affect the resolution of the developed pattern. Two factors are determined to be critical to pattern resolution, the initial crystallinity of the polymer, here poly(3-hexylthiophene) (P3HT), and the quality of the development solvent. We find that dopants diffuse more readily in highly crystalline films than in amorphous films of P3HT and that dopant diffusion reduces the fidelity of the resulting pattern. We also find that the choice of development solvent affects both the fidelity of the pattern and dopant distribution within the patterned polymer domains. Finally, we show that a dopant that diffuses more slowly than F4TCNQ in the P3HT film can be used to pattern the film with higher fidelity. These results together provide a road map for optimizing additive DISC patterning for any polymer/dopant pair.

36 MATERIALS SCIENCE↗

Copper adparticle enabled selective electrosynthesis of n-propanol

Here, the electrochemical reduction of carbon monoxide is a promising approach for the renewable production of carbon-based fuels and chemicals. Copper shows activity toward multi-carbon products from CO reduction, with reaction selectivity favoring two-carbon products; however, efficient conversion of CO to higher carbon products such as n-propanol, a liquid fuel, has yet to be achieved. We hypothesize that copper adparticles, possessing a high density of under-coordinated atoms, could serve as preferential sites for n-propanol formation. Density functional theory calculations suggest that copper adparticles increase CO binding energy and stabilize two-carbon intermediates, facilitating coupling between adsorbed *CO and two-carbon intermediates to form three-carbon products. We form adparticle-covered catalysts in-situ by mediating catalyst growth with strong CO chemisorption. The new catalysts exhibit an n-propanol Faradaic efficiency of 23% from CO reduction at an n-propanol partial current density of 11 mA cm –2 .

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Full spectrum light driven photocatalytic in-situ epitaxy of one-unit-cell Bi 2 O 2 CO 3 layers on Bi 2 O 4 nanocrystals for highly efficient photocatalysis and mechanism unveiling

In-situ epitaxial growth is a fascinating strategy to nicely couple two low dimensional semiconductors as highly efficient composite photocatalysts. Meanwhile, organic contaminants in the photocatalytic process are usually decomposed into greenhouse gas (CO 2 ) that can’t be reused. Herein, we reported a green full spectrum light (UV, visible and NIR lights) induced epitaxial growth strategy to synthesize highly efficient Bi 2 O 4 /Bi 2 O 2 CO 3 heterostructure photocatalyst by reusing waste carbon source, in which one-unit-cell Bi 2 O 2 CO 3 layers (1.0 nm) in-situ grew on the surface of Bi 2 O 4 nanocrystals during the photocatalytic degradation of rhodamine B (RhB) or phenol. More importantly, 13 C nuclear magnetic resonance (NMR) spectroscopy confirmed that the carbon element in Bi 2 O 2 CO 3 was from the photocatalytic degradation of organic contaminations. Furthermore, density functional theory (DFT) calculations confirm that the Bi 2 O 4 nanocrystals with exposed {-101} facets have the larger percentage of undercoordinated Bi atoms, which provided favorable conditions for the in-situ epitaxy of Bi 2 O 2 CO 3 during the photocatalytic reaction. Additionally, the increased charge density near the Fermi level resulted in improved photoresponsivity of Bi 2 O 4 /Bi 2 O 2 CO 3 composite and the coalescence of Bi 2 O 4 and Bi 2 O 2 CO 3 could favor the travel of photogenerated carriers from one to another owing to the close work functions for Bi 2 O 4 (4.295 eV) and Bi 2 O 2 CO 3 (4.410 eV). As we expected, the Bi 2 O 4 /Bi 2 O 2 CO 3 composite presented higher photocatalytic activity for phenol and ciprofloxacin (CIP) degradation than pure Bi 2 O 4 nanocrystals. The possible degradation pathway of CIP in aqueous solution and photocatalytic mechanism of Bi 2 O 4 /Bi 2 O 2 CO 3 composite were also proposed based on liquid chromatography mass spectrometer (LC–MS) analysis and experimental results. Furthermore, this work provides a green strategy for designing highly efficient photocatalysts.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

c-Myc-driven glycolysis via TXNIP suppression is dependent on glutaminase-MondoA axis in prostate cancer

Highlights: • c-Myc suppresses TXNIP transcription in a glutamine-dependent manner. • c-Myc induction of GLS1 is necessary for TXNIP suppression. • TXNIP represses glycolytic target genes broadly in c-Myc-driven cancers. • c-Myc and TXNIP levels are negatively associated in PCA tissues and predict patient outcome. Oncogenic c-Myc-induced metabolic reprogramming triggers cellular dependency on exogenous glucose and glutamine. Understanding how nutrients are used may provide new target for therapeutic intervention. We previously provided an alternate route to c-Myc-driven glucose metabolism via the repression of thioredoxin-interacting protein (TXNIP), which is a potent negative regulator of glucose uptake. Herein, we demonstrate that c-Myc suppression of TXNIP is predominantly through the activation of glutaminolysis via glutaminase (GLS1) in prostate cancer cells. Glutamine depletion blocked c-Myc-dependent reductions of TXNIP and its principal regulator MondoA transcriptional activity. Further, GLS1 inhibition by either siRNA or CB-839 resumed TXNIP expression that was repressed by c-Myc. The TXNIP promoter with mutant E-Box region, which was recognized by MondoA, failed to respond to c-Myc or GLS1, indicating c-Myc repression of TXNIP by GLS1 is predominantly through the blockage of MondoA activity. Especially, ectopic TXNIP expression decreased c-Myc-induce glucose uptake and lead to a broad range of glycolytic target gene suppressions. Thus TXNIP is a key adaptor for c-Myc-driven aerobic glycolysis. Supporting the biological significance of c-Myc and TXNIP, their reciprocal relationship are correlates with patient outcome and contributes to the aggressive phenotype in PCAs.

60 APPLIED LIFE SCIENCES↗

Nitrogen and sulfur co-doped porous carbon sheets for energy storage and pH-universal oxygen reduction reaction

Developing efficient electrocatalysts for energy storage and oxygen reduction reaction (ORR) is of great sig-nificance for the utilization of renewable energy. In particular, designing catalysts with both promising activityand long stability for ORR in pH-universal electrolytes still remain as a tremendous challenge. To tackle such aproblem, metal-free nitrogen and sulfur co-doped porous carbon sheet (NSPCS) was rationally designed in thiswork in order to integrate the two reported routes of enhancing the electrocatalytic activity of graphene. The as-prepared NSPCS has an onset potential of 0.89 V vs. RHE, and half-wave potential E1/2 ≈ 0.75 V during ORR inacidic solution, making it as the most active ORR catalyst. Moreover, the resulting NSPCS also shows a 0.03 Vpositive shift of half-wave potential than commercial Pt/C for ORR and excellent charge capacitive performancein alkaline media. Electron microscopy revealed high degree of defects on NSPCS surface. This, coupled withsynergistic doping effects of nitrogen and sulfur, optimized the active sites and charge transfer, rationalized theoutstanding performance in both oxygen reduction reactions and supercapacitors.Developing efficient electrocatalysts for energy storage and oxygen reduction reaction (ORR) is of great significance for the utilization of renewable energy. In particular, designing catalysts with both promising activity and long stability for ORR in pH-universal electrolytes still remain as a tremendous challenge. To tackle such a problem, metal-free nitrogen and sulfur co-doped porous carbon sheet (NSPCS) was rationally designed in this work in order to integrate the two reported routes of enhancing the electrocatalytic activity of graphene. The as-prepared NSPCS has an onset potential of 0.89 V vs. RHE, and half-wave potential E-1/2 approximate to 0.75 V during ORR in acidic solution, making it as the most active ORR catalyst. Moreover, the resulting NSPCS also shows a 0.03 V positive shift of half-wave potential than commercial Pt/C for ORR and excellent charge capacitive performance in alkaline media. Electron microscopy revealed high degree of defects on NSPCS surface. This, coupled with synergistic doping effects of nitrogen and sulfur, optimized the active sites and charge transfer, rationalized the outstanding performance in both oxygen reduction reactions and supercapacitors.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Discharge Permit-1845 Quarterly Status Report October 2018

Trichloroethene (TCE) and nitrate have been identified as constituents of concern in groundwater at the Sandia National Laboratories, New Mexico (SNL/NM) Technical Area (TA)-V Groundwater (TAVG) Area of Concern (AOC) based on detections above the U.S. Environmental Protection Agency (EPA) maximum contaminant level (MCL) in samples collected from monitoring wells. The EPA MCLs and the State of New Mexico drinking water standards for TCE and nitrate are 5 micrograms per liter and 10 milligrams per liter (as nitrogen), respectively. A phased Treatability Study/Interim Measure (TS/IM) of in-situ bioremediation (ISB) is being implemented to evaluate the effectiveness of ISB as a potential technology to treat the groundwater contamination at the TAVG AOC (New Mexico Environment Department [NMED] April 2016). The NMED Hazardous Waste Bureau (HWB) approved the Revised Treatability Study Work Plan (TSWP) (SNL/NM March 2016) in May 2016 (NMED May 2016). The SNL/NM Environmental Restoration Operations personnel are responsible for implementing the TS/IM of ISB at TAVG AOC in accordance with the Revised TSWP. Per the Revised TSWP, up to three injection wells (TAV-INJ1, TAV-INJ2, and TAV-INJ3) would be installed at TA-V in the vicinity of the highest contaminant concentrations detected in groundwater at monitoring wells LWDS-MW1, TAV-MW6, and TAV-MW10. The injection wells would be used to gravity-inject substrate solution and biodegradation bacteria to groundwater. The substrate solution consists of an inert tracer as well as essential food and nutrients for biostimulation. The substrate solution would be prepared in aboveground tanks. The TS/IM would be conducted in two phases: Phase I includes a pilot test followed by full-scale injection at the first injection well (TAV-INJ1); Phase II includes full-scale injections at the second and third injection wells (TAV-INJ2 and TAV-INJ3). The NMED Ground Water Quality Bureau (GWQB) requires a groundwater Discharge Permit (DP) for the operation of injection wells. NMED GWQB issued the DP-1845 to the U.S. Department of Energy/National Nuclear Security Administration (DOE/NNSA) for the SNL/NM TA-V Treatability Study injection wells on May 26, 2017 (NMED May 2017). The DP-1845 term started on May 30, 2017 and ends on May 30, 2022. Attachment A provides a copy of DP-1845. This quarterly report provides responses to DP-1845 Operating Conditions Terms and Conditions #3 through #8 and Monitoring and Reporting Terms and Conditions #10 through #17 for the April 1 to June 30, 2018 reporting period. The other Terms and Conditions are NMED statements of fact and do not require a response.

54 ENVIRONMENTAL SCIENCES↗

miR-7-5p acts as a tumor suppressor in bladder cancer by regulating the hedgehog pathway factor Gli3

Although important progresses have been made in the diagnosis and treatment of bladder cancer (BCa), the overall survival for patients with advanced BCa remains poor. It is necessary to uncover the molecular mechanism underlying the initiation and progression of bladder cancer. According to previous reports, mircoRNAs (miRNAs) can regulate tumorigenesis by targeting their downstream mRNAs. This study aims to explore and analyze a novel miRNA-mRNA axis which can regulate the progression of bladder cancer. Based on the microarray analysis, 182 mRNAs were found to be upregulated in BCa tissues. Gene oncology (GO) analysis and Kyoto Encyclopedia of Genes and Genomes (KEGG) analysis revealed that these upregulated mRNAs are related with hedgehog pathway. Gli3, an important factor of hedgehog pathway, belongs to these 182 upregulated mRNAs. Therefore, Gli3 was chosen to do further study. Kaplan-Meier analysis revealed that highly expressed Gli3 predicted unfavorable prognosis for patients with BCa. Results of functional experiments indicated the inhibitory effects of silenced Gli3 on cell proliferation, migration and EMT progress. Mechanically, Gli3 was the target mRNA of miR-7-5p in BCa cells. Finally, rescue assays were performed to validate the specific function of miR-7-5p/Gli3 axis in BCa progression. According to all data, we concluded that miR-7-5p acts as a tumor suppressor in BCa by downregulating Gli3.

60 APPLIED LIFE SCIENCES↗

Unconventional Relation between Charge Transport and Photocurrent via Boosting Small Polaron Hopping for Photoelectrochemical Water Splitting

Doping in semiconductor photoelectrodes controls defect formation and carrier transport that critically determine the device performance. Here we report an unconventional carrier transport relation that is tuned by extrinsic molybdenum (Mo) doping in BiVO 4 photoanodes. Using the single-crystalline thin film approach, we identify that Mo doping significantly condenses the optimization regime between carrier transport and photon collection. For Mo-doped BiVO 4 films, an unprecedentedly thin layer (50 nm), less than one-third of the pristine BiVO 4 thickness, delivers larger photocurrents by overcoming the charge transport limitation, representing a regime not covered in conventional models. We provide direct evidence that Mo doping improves electron transport by boosting not only the donor density but also the electron mobility in the form of a small polaron, with the latter applying substantial impact on the photoelectrochemical performance. Density functional theory calculations reveal that fully ionized Mo dopants establish a strong electrostatic interaction with a small polaron, which helps reduce its hopping barrier by minimizing the local lattice expansion. Here, our results deliver mechanistic insights on the interplay between extrinsic doping and carrier transport, and provide guidance in developing advanced semiconductor photoelectrodes.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

A facile and low-cost synthesis of MnOx/Mn2NNC nanohybrid as an advanced oxygen reduction electrocatalyst

Highlights: • We demonstrate a facile route to fabricate a novel MnO{sub x}/Mn{sub 2}NNC hybrid. • MnO{sub x}/Mn{sub 2}NNC displays an excellent ORR activity. • MnO{sub x}/Mn{sub 2}NNC affords overwhelmingly better durability than 20 wt% Pt/C. - Abstract: We demonstrate a one-step, low-cost and easily scalable pyrolysis route to fabricate a novel MnO{sub x}/Mn{sub 2}NNC nanohybrid with MnO{sub x}/Mn{sub 2}N nanoparticles (20–30 nm) anchored on the wrinkled N-doped carbon nanosheets (denoted as NC). MnO{sub x}/Mn{sub 2}NNC displays a remarkably higher ORR activity than that of NC, suggesting that the MnO{sub x}/Mn{sub 2}N nanoparticles play an important role in enhancing the ORR activity. Furthermore, MnO{sub x}/Mn{sub 2}NNC exhibits overwhelmingly better durability than commercial 20 wt% Pt/C, to be specific, 93.7% current retention after continuous operation for 24,000 s, while 59.7% for 20 wt% Pt/C.

77 NANOSCIENCE AND NANOTECHNOLOGY↗