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Although composite solid-state electrolytes (CSEs) are considered promising ionic conductors for high-energy lithium metal batteries, their unsatisfactory ionic conductivity, low mechanical strength, poor thermal stability, and narrow voltage window limit their practical applications. We have prepared a new lithium superionic conductor (Li-HA-F) with an ultralong nanofiber structure and ultrahigh room-temperature ionic conductivity (12.6 mS cm-1). When it is directly coupled with a typical poly(ethylene oxide)-based solid electrolyte, the Li-HA-F nanofibers endow the resulting CSE with high ionic conductivity (4.0 × 10-4 S cm-1 at 30 °C), large Li+ transference number (0.66), and wide voltage window (5.2 V). Detailed experiments and theoretical calculations reveal that Li-HA-F supplies continuous dual-conductive pathways and results in stable LiF-rich interfaces, leading to its excellent performance. Moreover, the Li-HA-F nanofiber-reinforced CSE exhibits good heat/flame resistance and flexibility, with a high breaking strength (9.66 MPa). As a result, the Li/Li half cells fabricated with the Li-HA-F CSE exhibit good stability over 2000 h with a high critical current density of 1.4 mA cm-2. Furthermore, the LiFePO4/Li-HA-F CSE/Li and LiNi0.8Co0.1Mn0.1O2/Li-HA-F CSE/Li solid-state batteries deliver high reversible capacities over a wide temperature range with a good cycling performance.
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Ammonium (NH4+) is a key inorganic nitrogen source in cellular amino acid biosynthesis. The coupling of transcriptional and posttranslational regulation of AMMONIUM TRANSPORTER (AMT) ensures that NH4+ acquisition by plant roots is properly balanced, which allows for rapid adaptation to a variety of nitrogen conditions. Here, we report that phospholipase D (PLD)-derived phosphatidic acid (PA) interacts with AMT1;1 to mediate NH4+ uptake in Arabidopsis (Arabidopsis thaliana). We examined pldα1 pldδ-knockout mutants and found that a reduced PA level increased seedling growth under nitrogen deficiency and inhibited root growth upon NH4+ stress, which was consistent with the enhanced accumulation of cellular NH4+. PA directly bound to AMT1;1 and inhibited its transport activity. Mutation of AMT1;1 R487 to Gly (R487G) resulted in abolition of PA suppression and, subsequently, enhancement of ammonium transport activity in vitro and in vivo. Observations of AMT1;1-GFP showed suppressed endocytosis under PLD deficiency or by mutation of the PA-binding site in AMT1;1. Endocytosis was rescued by PA in the pldα1 pldδ mutant but not in the mutant AMT1;1R487G-GFP line. Together, these findings demonstrated PA-based shutoff control of plant NH4+ transport and point to a broader paradigm of lipid-transporter function.
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Compuestos de Amonio , Proteínas de Arabidopsis , Arabidopsis , Compuestos de Amonio/farmacología , Compuestos de Amonio/metabolismo , Arabidopsis/metabolismo , Proteínas de Arabidopsis/genética , Proteínas de Arabidopsis/metabolismo , Proteínas de Transporte de Membrana/metabolismo , Nitrógeno/metabolismo , Ácidos Fosfatidicos/metabolismo , Raíces de Plantas/metabolismoRESUMEN
A key component of scientific communication is sufficient information for other researchers in the field to reproduce published findings. For computational and data-enabled research, this has often been interpreted to mean making available the raw data from which results were generated, the computer code that generated the findings, and any additional information needed such as workflows and input parameters. Many journals are revising author guidelines to include data and code availability. This work evaluates the effectiveness of journal policy that requires the data and code necessary for reproducibility be made available postpublication by the authors upon request. We assess the effectiveness of such a policy by (i) requesting data and code from authors and (ii) attempting replication of the published findings. We chose a random sample of 204 scientific papers published in the journal Science after the implementation of their policy in February 2011. We found that we were able to obtain artifacts from 44% of our sample and were able to reproduce the findings for 26%. We find this policy-author remission of data and code postpublication upon request-an improvement over no policy, but currently insufficient for reproducibility.
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A porous g-C3N4 nanosheet containing nitrogen defects (D-g-C3N4) was synthesized by using a one-step polymerization process in an atmosphere produced via the decomposition of ammonium persulfate. The photocatalytic removal rate of D3-g-C3N4 for meropenem (MER) is 7.45-fold higher than the one of a conventional g-C3N4 sample. The sample mineralization increases from 27% to 52% when the defects are generated. The position of the N defects was inferred via XPS, element analysis and ESR. The introduction of the N2C defects leads to the formation of a midgap state that suppresses the photoexcited carrier recombination. In addition, several environmental factors were simulated during the MER degradation including the initial concentration of MER, of humic acid (HA), and of the common anions and cations. The analysis of the Fukui function combined with LC-Q-TOF-MS predicted the probable degradation path of MER. Its main channel includes the breaking of the ß-lactam ring and of the C-S bond, and the shedding of the carboxyl group and the amino group. Moreover, the toxicity of the intermediates was acquired via USEPA.
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Nitrógeno , Catálisis , Teoría Funcional de la Densidad , Meropenem , PorosidadRESUMEN
A novel and effective route for preparing phenol formaldehyde resin grafted reduced graphene oxide (rGO-g-PF) electrode materials with highly enhanced electrochemical properties is reported. In order to prepare rGO-g-PF, hydroxymethyl-terminated PF is initially grafted to graphene oxide (GO) via esterification reaction. Subsequently, the grafted GO is reduced by the carbonization process under an inert gas atmosphere. The covalent linkage, morphology, thermal stability and electrochemical properties of rGO-g-PF are systematically investigated by Fourier transform infrared spectroscopy, scanning electron microscopy, thermal gravimetric analysis, differential scanning calorimetry and a variety of electrochemical testing techniques. In the constructed architecture, the amorphous carbon shell can inhibit the co-intercalation of solvated lithium ion and avoid partial exfoliation of the graphene layers, thus effectively reducing the irreversible capacity and preserving the structural integrity. Meanwhile, the carbon coating layer leading to a decreased thickness of SEI film can improve the conductivity of electrode materials. As a result, the rGO-g-PF electrode exhibits impressive high cycling stability at various large current densities (376.5 mA h g(-1) at 50 mA g(-1) for 250 cycles, 337.8 mA h g(-1) at 200 mA g(-1) and 267.8 mA h g(-1) at 1 A g(-1) for 200 cycles), in combination with high rate capability.
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In order to gain a profound understanding of the fate of pollutants in advanced oxidation processes (AOPs), this study analyzed the electron contribution of pollutants qualitatively and quantitatively which rarely reported before. The rich electron transfer system was constructed by mesoporous carbon nitride (MCN) coupling with persulfate (PS) driven by visible light and the sulfanilamide antibiotics (SULs) were used as target contaminants. Firstly, the qualitative analysis of electron transfer in the system was confirmed systematically. The electron flow direction tested by i-t curves indicated that PS absorbed electrons, while SULs released electrons. The flow rate of electrons was also accelerated after the addition of SULs. The fitting curve between the kinetics and the peak potential difference tested by CV curve showed that the larger potential difference, the slower rate of oxidative degradation. Secondly, the quantification of electron transfer was achieved through theoretical calculations to simulate the interactions of the 'catalyst-oxidant-antibiotic' system. After the addition of SULs, the adsorption energy of the 'catalyst-oxidant-antibiotic' system was enhanced and the bond length of the peroxide bond was stretched. Notably, the electron transfer analysis results showed that the charge of SULs was around 0.032-0.056e, indicating that SULs pollutants played the role of electron contributors in the system. The oxidative degradation pathway included the direct cracking of S-N bond, shedding of marginal groups, ring-opening and hydroxyl addition reaction. This study clarified the electronic contribution of SULs in the oxidation system, providing necessary theoretical supplement for the analysis of the transformation of pollutants in AOPs.
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In the study, an efficient '1 + 1 > 2' synergistic coupling system driven by visible light consisting of mesoporous g-C3N4 (MCN) and persulfate (PS)was constructed. The free radical transformation, electron transfer and non-covalent interaction between the MCN layer and PS in the system were explored via experiments and DFT calculations. The similarity for the fate of the seven ß-lactam antibiotics with typical structures in the oxidation system was studied systematically in depth. First, the consistencies and differences of the seven antibiotics were summarized from three aspects: three-dimensional structures, electron cloud distributions, and the vulnerable sites. Notably, the selective differential degradation of ß-lactam antibiotics in the MCN/PS system was speculated to be related with the molecular ionization potential (MIP), as a key index to describe the difficulty of oxidation. The distribution relationship between MIP and the oxidation kinetic constant (K) was explored and showed the following trend: a higher MIP indicates a weaker ability to provide electrons, and this leads to a greater resistance to oxidative degradation. In total, four main oxidation pathways of ß-lactam antibiotics were systematically summarized combining HPLC-QTOF-MS and the simplified Fukui function calculation. The toxicity assessment of intermediate products provided by the T.E.S.T software of USEPA also shows a decreasing trend in the oxidation process. In the end, the superior practicability and stability of the MCN/PS system was verified by complex environment simulation and cyclic test. This research clarified the selective differential degradation mechanism of ß-lactam antibiotics and provided a possible idea for the effective removal of refractory organic pollutants in water.
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Luz , Contaminantes Químicos del Agua , Antibacterianos , Cinética , Oxidación-Reducción , beta-LactamasRESUMEN
The magnetic manipulation of droplets is one of the emerging magnetofluidic technologies that integrate multiple disciplines, such as electromagnetics, fluid mechanics and so on. The directly driven droplets are mainly composed of ferrofluid or liquid metal. This kind of magnetically induced droplet manipulation provides a remote, wireless and programmable approach beneficial for research and engineering applications, such as drug synthesis, biochemistry, sample preparation in life sciences, biomedicine, tissue engineering, etc. Based on the significant growth in the study of magneto droplet handling achieved over the past decades, further and more profound explorations in this field gained impetus, raising concentrations on the construction of a comprehensive working mechanism and the commercialization of this technology. Current challenges faced are not limited to the design and fabrication of the magnetic field, the material, the acquisition of precise and stable droplet performance, other constraints in processing speed and so on. The rotational devices or systems could give rise to additional issues on bulky appearance, high cost, low reliability, etc. Various magnetically introduced droplet behaviors, such as deformation, displacement, rotation, levitation, splitting and fusion, are mainly introduced in this work, involving the basic theory, functions and working principles.
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Campos Magnéticos , Ingeniería de Tejidos , Fenómenos Electromagnéticos , Reproducibilidad de los ResultadosRESUMEN
The environmental hazards of antibiotics and the resulting antibiotic-resistant bacteria (ARB) have attracted more and more attention. In this study, an efficient synergistic system constructed by vacancy g-C3N4 (CNV0.8) and persulfate (PS) showed excellent oxidation performance to degrade aztreonam (AZT) and Escherichia coli (E. coli) screened from wastewater treatment plant (WWTP), as the typical ß-lactam antibiotic and ARB. As the recombination of electron and hole was effectively inhibited and the interaction with PS was enhanced after the introduction of defects, CNV0.8 showed superior PS activation ability compared with bulk-g-C3N4 (BCN). The synergistic mechanism was systematically analyzed at three levels step by step. Firstly, the conversion of reactive oxygen radicals (ROSs) was studied using electron spin resonance (ESR) and quenching experiments. Then based on the DFT simulation, the enhancement of adsorption energy between catalysts and PS from -8.924 eV (BCN) to -11.190 eV (CNV0.8) and the elongation of O-O bond in PS (from 1.496 Å to 1.505 Å) indicated CNV0.8 had better activation performance for PS compared with BCN. The electron transfer results observed by deformation charge density showed that more electrons could be transferred from the CNV0.8 layer to the surrounding of PS for its own activation in the synergistic mechanism. Thirdly, the noncovalent interaction of PS/CNV0.8 belonged to the region of van der Waals force which was defined by the reduced density gradient (RDG) analysis. The intermediate products in the degradation of AZT were first studied in detail using Fukui function calculations and HPLC-QTOF-MS analysis. Subsequently, the environmental practicability of the oxidation system was investigated through wastewater simulation. This research provides a possible strategy for the effective removal of micropollutants and promotes the development of the sulfate radical-advanced oxidation processes (SR-AOPs) in the field of wastewater treatment.
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Electrones , Contaminantes Químicos del Agua , Antagonistas de Receptores de Angiotensina , Inhibidores de la Enzima Convertidora de Angiotensina , Antibacterianos/farmacología , Escherichia coli , Oxidación-Reducción , Contaminantes Químicos del Agua/análisisRESUMEN
Coal is well known as the primary energy consumption in China, and the coal chemical industry (CCI) can serve as an important source of volatile organic compounds (VOCs) emissions. However, the characteristics of VOCs emitted from CCI along with their environmental consequences are still poorly understood. To pin down this, an intensive field campaign was carried out at a typical CCI city in northwestern China (Yulin) from February 26 to March 7, 2021. Results showed that VOC compositions in Yulin were distinct from those in the megacities of China as well as in the typical oilfields over the world. The concentration of naphthalene (1.6 ± 1.1 ppbv), an important byproduct of CCI, was significantly higher than that in other cities (<0.2 ppbv). Positive matrix factorization (PMF) model analysis revealed that the direct contribution of the CCI source for VOC emissions is 8.8 ± 1.8%. More importantly, these VOCs emitted from the CCI can account for 17.9 ± 6.8% of ozone (O3) formation potential and 16.9 ± 7.4% of OH reactivity of VOCs, suggesting the significant impacts of the CCI on the air quality and atmospheric oxidizing capacity. During the observation, a rapid increase in O3 concentration after a snowfall was encountered. The changing rate of O3 concentration in the daytime was significantly higher than in its peripheral cities. The increased O3 formation was partially attributed to the CCI, and this enhancement can be further magnified by snow cover due to the increment of surface albedo. These findings deepen the understanding of the characteristics and air quality impact of VOCs related to the CCI and provide valuable insights for the development of air quality control measures in the region influenced by intensive coal chemical production.
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Contaminantes Atmosféricos , Ozono , Compuestos Orgánicos Volátiles , Contaminantes Atmosféricos/análisis , Industria Química , China , Ciudades , Carbón Mineral/análisis , Monitoreo del Ambiente/métodos , Ozono/análisis , Emisiones de Vehículos/análisis , Compuestos Orgánicos Volátiles/análisisRESUMEN
Microbial fuel cells (MFCs) are devices that treat sewage and generate electricity. Recent researches have demonstrated that the characteristics of carbon precursors can tremendously influence the performance of the MFC cathode. Carbon nanomaterials with good crystallinity as well as high specific surface area (e.x., graphene and carbon nanotube) can not only accelerate charge transport but also afford a good dispersion of catalytic active components, leading to high MFC performance. On these bases, the preparation of highly-active Fe-N/C catalysts using different carbon substrates are mainly discussed in this review. It is pointed out that increasing the surface area and conductivity as well as elevating the density of active sites to reduce the oxygen reduction overpotential is still the emphasis of the current works. At present, although the researchers have made some progress, the output power density is far from meeting the actual application needs.
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Fuentes de Energía Bioeléctrica , Electrodos , Hierro , Nitrógeno , Oxidación-Reducción , OxígenoRESUMEN
Through one-step pyrolysis, non-noble-metal oxygen reduction reaction (ORR) electrocatalysts were constructed from ferric trichloride, melamine, and graphene nanoribbon@carbon nanotube (GNR@CNT), in which a portion of the multiwall carbon nanotube is unwrapped/unzipped radially, and thus graphene nanoribbon is exposed. In this study, Fe-N/GNR@CNT materials were used as an air-cathode electrocatalyst in microbial fuel cells (MFCs) for the first time. The Fe-N/C shows similar power generation ability to commercial Pt/C, and its electron transfer number is 3.57, indicating that the ORR process primarily occurs with 4-electron. Fe species, pyridinic-N, graphitic-N, and oxygen-containing groups existing in GNR@CNT frameworks are likely to endow the electrocatalysts with good ORR performance, suggesting that a GNR@CNT-based carbon supporter would be a good candidate for the non-precious metal catalyst to replace Pt-based precious metal.
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Phenolic carbon felt (PCF) is a three-dimensional material with a simple manufacturing process and low cost. To investigate the application of PCF as an anode material for use in microbial fuel cells (MFCs), we employed PCF as the anode material for the first time in MFCs that were carbonized at different temperatures. The relationship between the intrinsic characteristics and the electrochemical performance of different PCFs was also analyzed. Here, we obtained the best power generation with a power density of up to 2600 mW/m2 when PCF was heated to 900 °C (PCF-900); this power generation was much higher than that of the commercial carbon felts. From SEM images, we found that the biofilm growth of PCF-900 was quite uniform. This may result from the higher surface electropositivity of PCF-900 and increased electrostatic attraction between the microorganisms and PCF. We also analyzed the conductivity, specific surface area, functional groups, and surface charge of the PCF anode. Under the synergistic effect of these intrinsic properties, PCF-900 showed good biocompatibility for the adhesion of microorganisms and high electron transfer efficiency. In addition, PCF was easily prepared in different sizes. Thus, it could be a promising material for the application of scale-up MFCs.
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Fuentes de Energía Bioeléctrica , Fibra de Carbono/química , Fenoles/química , Adhesión Bacteriana , Biopelículas/crecimiento & desarrollo , Conductividad Eléctrica , Electrodos , Cinética , Propiedades de Superficie , TemperaturaRESUMEN
Herein, carbon brush cylindrical microbial fuel cell is constructed to decrease internal resistance and increase electricity production. The application of cylindrical single-chamber microbial fuel cell gives full play to the role of anode carbon brush and increases contact with surrounding oxygen by enlarging the surface area of the cathode. Both cylindrical design and P. aeruginosa inoculation in anode have positive effects on power output of microbial fuel cells. Changing the configuration from cubic to cylindrical resulted in a substantial reduction in internal resistance from 127.21â¯Ω to 49.66â¯Ω. Meanwhile, the cylindrical microbial fuel cell inoculated with mixed anaerobic bacteria exhibits power overshoot, and the dissolved oxygen in the electrolyte is raised. Thus, we also select P. aeruginosa inoculation in cylindrical reactor, where the maximum power density is increased to 3322⯱â¯38â¯mWâ¯m-2 and internal resistance is reduced to 34.0⯱â¯1.1â¯Ω, and then power overshoot is improved. Thus, P. aeruginosa showed better electrogenic performance than anaerobic mixtures. In addition, chemical oxygen demand removal efficiencies (about one cycle) of the three microbial fuel cells are similar, but the cylindrical cell handles about 0.7 times of sewage more than the cubic cell showing that cylindrical microbial fuel cell has a higher capacity of sewage treatment.
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Fuentes de Energía Bioeléctrica , Pseudomonas aeruginosa/metabolismo , Fuentes de Energía Bioeléctrica/microbiología , Análisis de la Demanda Biológica de Oxígeno , Electricidad , Electrodos , Oxígeno/metabolismo , Aguas del Alcantarillado/microbiologíaRESUMEN
This work proposes a simple and efficient approach for the formation of short carbon nanotubes (CNTs) on graphene sheets. This paper investigates the effect of heat treatment time on the morphology of CNTs. The mechanism of the growth and disappearance of CNTs are also investigated. Graphene is added into ferric trichloride (FeCl3)-melamine solution to obtain a suspension. The suspension is dried with stirring, followed by a carbonization process under N2 atmosphere, resulting in the formation of CNTs on graphene sheets. The thus-prepared carbon material can be used as a kind of durable and efficient non-precious metal oxygen reduction reaction (ORR) electrocatalyst. The ORR activity of the catalyst with favorable performance is characterized and compared with a commercial Pt/C catalyst. The results show that the ORR electron transfer number of Fe-N/G with CNTs is 3.91 ± 0.02. The Fe-N/G-MFC achieves a maximum power density of 1210 ± 23 mW m-2, which is much higher than Pt/C-MFC (1080 ± 20 mW m-2). It demonstrates that Fe-N/G materials with CNTs can be a type of promising highly efficient catalyst and can enhance ORR performance of MFCs. Besides, the reason for the disappearance of CNTs we investigated in this study may provide some ideas for the study of loading metal oxide catalysts on CNTs.
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Microbial fuel cells (MFCs) are a promising energy-positive wastewater treatment technology, however, the system's cost-effectiveness has been overlooked. In this study, two new anode materials - hard felt (HF) and carbon foam (CF) - were evaluated against the standard graphite brush (GB) to determine if using inexpensive materials with less than ideal properties can achieve more cost-effective treatment than high-cost, high-performing materials. Using domestic wastewater as the substrate, power densities for the GB, HF and CF-MFCs were 393, 339 and 291 mW m(-2) normalized by cathodic surface area, respectively. Higher power densities correlated with larger anodic surface areas and anodic current densities but not with electrical conductivity. Cyclic voltammetry revealed that redox systems used for extracellular electron transport in the GB, HF and CF-MFCs were similar (-0.143 ± 0.046, -0.158 ± 0.004 and -0.100 ± 0.014 V vs. Ag/AgCl) and that the electrochemical kinetics of the MFCs showed no correlation with their respective electrical conductivity. 16S rRNA sequencing showed the GB, HF and CF microbial community compositions were not statistically different while organic removal rates were nearly identical for all MFCs. The HF-MFC generated a power output to electrode cost (W $(-1)) 1.9 times greater than the GB-MFC, despite producing 14% less power and 15% less anodic current, while having 2.6 times less anodic surface area, 2.1 times larger charge transfer resistance and an electrical conductivity three orders of magnitude lower. The results demonstrate that inexpensive materials are capable of achieving more cost-effective treatment than high-performing materials despite generating lower power when treating real wastewater.
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Fuentes de Energía Bioeléctrica , Carbono/química , Aguas Residuales/microbiología , Purificación del Agua/métodos , Biodegradación Ambiental , Fuentes de Energía Bioeléctrica/economía , Fuentes de Energía Bioeléctrica/microbiología , Análisis Costo-Beneficio , Electrodos , ARN Ribosómico 16S , Aguas Residuales/química , Purificación del Agua/economía , Purificación del Agua/instrumentaciónRESUMEN
We have fabricated CuO@TiO2 nanocable arrays by a facile method involving in situ thermal oxidation of Cu foil and coating of tetrabutyl titanate solution. The structure of the nanocables has been investigated by various techniques to comfirm that the cores are mainly crystalline monoclinic CuO, and the shells are crystalline tetragonal anatase TiO2. When used as an anode material for lithium-ion batteries, the nanoconfinement effect plays an important role in improving the lithium-ion storage preformance: the lithiation will be confined in one-dimensional space of TiO2 nanotubes to limit the pulverization of CuO, and the phase interface will cause an interfacial adsorption to enrich more lithium ions at some level. Benefiting from the nanoconfinement effect and interfacial adsorption, the reversible capacity does not fade, but rather increases gradually to 725 mAh g(-1) after 400 cycles at a current density of 60 mA g(-1), superior to the theoretical capacity of CuO.
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Journal policy on research data and code availability is an important part of the ongoing shift toward publishing reproducible computational science. This article extends the literature by studying journal data sharing policies by year (for both 2011 and 2012) for a referent set of 170 journals. We make a further contribution by evaluating code sharing policies, supplemental materials policies, and open access status for these 170 journals for each of 2011 and 2012. We build a predictive model of open data and code policy adoption as a function of impact factor and publisher and find higher impact journals more likely to have open data and code policies and scientific societies more likely to have open data and code policies than commercial publishers. We also find open data policies tend to lead open code policies, and we find no relationship between open data and code policies and either supplemental material policies or open access journal status. Of the journals in this study, 38% had a data policy, 22% had a code policy, and 66% had a supplemental materials policy as of June 2012. This reflects a striking one year increase of 16% in the number of data policies, a 30% increase in code policies, and a 7% increase in the number of supplemental materials policies. We introduce a new dataset to the community that categorizes data and code sharing, supplemental materials, and open access policies in 2011 and 2012 for these 170 journals.