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At least 253 records · Page 14

Bio‐Inspired Cascade Photocatalysis on Fe Single‐Atom Carbon Nitride Upcycles Plastic Wastes for Effective Acetic Acid Production

Plastic imposes a critical threat to the environment, ecosystems, and human health because of the low utilization efficiency of plastics. Here, we demonstrate a sustainable, highly efficient cascade photocatalysis for upcycle plastics to value-added acetic acid using Fe single-atom catalysts (Fe@C 3 N 4 SAC) at ambient conditions. Inspired by Phanerochaete chrysosporium microbial, the defective Fe@C 3 N 4 SAC acts as a bifunctional cascade photocatalyst for both Fenton-like and CO 2 reduction reactions. During the reaction, hydroxyl radicals (*OH) form and subsequently oxidize plastics into CO 2 intermediates. These CO 2 intermediates are then photo-reduced to CH 3 COOH on the same catalyst via cascade photocatalysis. The mechanism is confirmed by in situ multimodal microscopy and spectroscopies, with density functional theory calculations. A state-of-art CH 3 COOH yield of 63.8 mg h −1 gcat −1 from PVC, 12.7 mg h −1 gcat −1 from PE, 5.4 mg h −1 gcat −1 from PET, and 5.3 mg h −1 gcat −1 from PP are directly obtained under AM1.5G solar irradiation and further validated under real sunlight (≈0.6 sun), achieving 5.6 mg h −1 gcat −1 from PET, using low-cost Fe@C 3 N 4 SAC in a sealed reactor by enhancing the photon transport and utilization efficiency. The techno-economic analysis shows it is promising to practically mitigate plastic based on broader social welfare assessments.

cascade photocatalysis↗

Preface to Special Issue of ChemSusChem on Lignin Valorization: From Theory to Practice

In this Editorial, Guest Editors Run-Cang Sun, Joseph S. M. Samec, and Arthur J. Ragauskas introduce the Special Issue of ChemSusChem on Lignin Valorization: From Theory to Practice. Here, the significance of and enormous challenges for the utilization of lignin are reviewed, and the contents of the Special Issue with highly interesting contributions from scientists around the world are outlined.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

High-efficiency single-junction p-i-n GaAs solar cell on roll-to-roll epi-ready flexible metal foils for low-cost photovoltaics

We demonstrate the fabrication and characterization of high-efficiency, single-junction p-i-n GaAs solar cells, on flexible metal foil with epi-ready buffer via roll-to-roll fabrication. Single-junction p-i-n GaAs solar cells were fabricated using metal–organic chemical vapor deposition (MOCVD). Furthermore, an efficiency greater than 13% was obtained at 1 sun, which is the highest reported efficiency on GaAs photovoltaics directly deposited on metal tapes. This exceeds our previously reported study showcasing 11.5% efficiency on single-junction p-n solar cell structure. Improved morphology of p-i-n structure compared with p-n is explained by atomic force microscopy (AFM), scanning electron microscopy (SEM), and helium ion microscopy (HIM) measurements. Time-of-flight secondary ion mass spectrometry (TOF-SIMS) analysis showed reduced Zn diffusion in p-i-n cell compared with the p-n cell. We attribute the improvement in efficiency of p-i-n cells on flexible metal tapes to the quality of the junction, surface morphology, controlled diffusion of species within the active layers, and increase in absorption due to the optimized intrinsic layer thickness.

14 SOLAR ENERGY↗

Seed‐Assisted Growth for Scalable and Efficient Perovskite Solar Modules

Perovskite solar modules (PSMs) have shown remarkable photovoltaic potentials, but they still suffer from large power conversion efficiency (PCE) loss on scale‐up and instability due to inferior uniformity and crystallization over large areas. Herein, the scalable production of efficient and stable PSMs using a suite of all‐scalable fabrication methods featuring a two‐step blade/dip‐coating approach to deposit the perovskite absorber layer is demonstrated. Rubidium chloride is introduced to embed (PbI 2 ) 2 RbCl complex seeds in the first‐deposited PbI 2 precursor, which assists in uniform crystallization of the perovskite layer with high crystallinity and reduced defect density over large areas. Following the optimization of RbCl additives, a champion PSM with 17.9% PCE on a 7.6 × 7.6 cm 2 substrate with a 37 cm 2 aperture area is achieved. Moreover, the RbCl‐incorporated PSMs demonstrate excellent reproducibility and stability under continuous 1 sun illumination. This work shows that the two‐step blade/dip coating is a promising method for producing high‐efficiency and stable PSMs on an industrially relevant scale.

Energy & Fuels↗

ELM Suppression by Boron Powder Injection and Comparison with Lithium Powder Injection on EAST

Type I edge-localized modes (ELMs) in the Experimental Advanced Superconducting Tokamak (EAST) were completely suppressed via boron powder injection into the X-point region of an upper-single null configuration over a wide range of operating conditions (2.8 < P aux < 7.5 MW, 3.8 × 10 19 < n e < 6 × 10 19 m -3 , RF-only and RF + NBI heating scenarios, both grad-B drift directions, and even He ion majority plasmas) (Sun et al. in Nucl. Fusion, 2020). A window of edge B concentration for stable long pulse operation was identified: too low and ELMs return, too high and the discharge suffers radiative collapse. The injection of boron powder above the minimum for ELM suppression coincided with the occurrence of an edge harmonic oscillation detected in magnetics (both on the high-field side and low-field side), in AXUV diodes near the upper X-point, divertor Dα emission, and in a range of other diagnostics (Diallo et al. in: Proceedings of 2020 IAEA fusion energy conference, 2021). Furthermore, no harmonic oscillation was observed when ELMs were present, and stored energy was slightly increased at constant density during ELM suppression. Core tungsten emission during ELM suppression either increased or decreased relative to ELMy H-mode, but the W emission was maintained at acceptable levels. The threshold B injection rate was measured for several conditions, and found to increase with heating power. Li powder injection into comparable discharges also resulted in a short phase of ELM suppression, but density and stored energy both decreased due to the strong pumping effect of lithium; no edge harmonic oscillation was observed with Li injection, indicating that the ELM suppression mechanisms differ. The new set of B-seeded, ELM-suppressed discharges exhibited certain characteristics of quiescent H-mode (Burrell et al. in Phys Plasmas 8:2153, 2001), but did not require high shear, counter beams, etc. The wide operating window and compatibility with RF-only discharges paves the way for future experiments targeting long pulse H-mode discharges with complete ELM suppression.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Mineral detection of neutrinos and dark matter. A whitepaper

Minerals are solid state nuclear track detectors — nuclear recoils in a mineral leave latent damage to the crystal structure. Depending on the mineral and its temperature, the damage features are retained in the material from minutes (in low-melting point materials such as salts at a few hundred °C) to timescales much larger than the 4.5 Gyr-age of the Solar System (in refractory materials at room temperature). The damage features from the O (50) MeV fission fragments left by spontaneous fission of 238U and other heavy unstable isotopes have long been used for fission track dating of geological samples. Laboratory studies have demonstrated the readout of defects caused by nuclear recoils with energies as small as O (1) keV. This whitepaper discusses a wide range of possible applications of minerals as detectors for E R ≳ O (1) keV nuclear recoils: Using natural minerals, one could use the damage features accumulated over O (10) Myr–O (1) Gyr to measure astrophysical neutrino fluxes (from the Sun, supernovae, or cosmic rays interacting with the atmosphere) as well as search for Dark Matter. Using signals accumulated over months to few-years timescales in laboratory-manufactured minerals, one could measure reactor neutrinos or use them as Dark Matter detectors, potentially with directional sensitivity. Research groups in Europe, Asia, and America have started developing microscopy techniques to read out the O (1)–O (100) damage features in crystals left by O (0.1)–O (100) keV nuclear recoils. We report on the status and plans of these programs. Furthermore, the research program towards the realization of such detectors is highly interdisciplinary, combining geoscience, material science, applied and fundamental physics with techniques from quantum information and Artificial Intelligence.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Characterizing leaf-scale fluorescence with spectral invariants

Sun-induced chlorophyll fluorescence (SIF) is increasingly recognized as a non-destructive probe for tracking terrestrial photosynthesis. Emerging developments in spectral invariants theory provide an innovative and efficient approach for representing SIF radiative transfer processes at the canopy scale. However, modeling leaf-scale fluorescence based on the spectral invariants properties (SIP) remains underexplored. In this study, the spectral invariants theory is employed for the first time to model the leaf-scale total, backward and forward fluorescence (leaf-SIP SIF). The leaf-SIP SIF model separates the leaf-scale radiative transfer process into two distinct components: the wavelength-dependent one associated with leaf biochemical properties, and the wavelength-independent component linked to leaf structural characteristics. The leaf structure-related effects are characterized by two spectrally invariant parameters: the photon recollision probability (p) and the scattering asymmetry parameter (q), which are parameterized using the directly measurable leaf dry matter. Evaluation against field measurements shows that the proposed leaf-SIP SIF model has a good performance, with coefficient of determination (R 2 ) of 0.89, 0.89, 0.90 and root mean squared errors (RMSE) of 1.28, 0.69, 0.74 Wm -2 µm -1 sr -1 , respectively for the total, backward, and forward fluorescence (660–800 nm). The leaf-SIP SIF model with a more concise formulation demonstrates comparable performance with the widely used Fluspect model. Further, the leaf-SIP SIF model provides a simple and efficient approach for simulating leaf-scale fluorescence, with the potential to be integrated into a unified SIP-based model framework for simulating the radiative transfer processes across the soil-leaf-canopy-atmosphere continuum.

59 BASIC BIOLOGICAL SCIENCES↗

Quantitative analyses of products and rates in polyethylene depolymerization and upcycling

Depolymerization and upcycling are promising approaches to managing plastic waste. However, quantitative measurements of reaction rates and analyses of complex product mixtures arising from depolymerization of polyolefins constitute significant challenges in this emerging field. Here, we detail techniques for recovery and analysis of products arising from batch depolymerization of polyethylene. We also describe quantitative analyses of reaction rates and products selectivity. This protocol can be extended to depolymerization of other plastics and characterization of other product mixtures including long-chain olefins. For complete details on the use and execution of this protocol, please refer to Sun et al.

Lee, Yu-Hsuan↗

Diamine chelates for increased stability in mixed Sn–Pb and all-perovskite tandem solar cells

Perovskite tandem solar cells show promising performance but non-radiative recombination and its progressive worsening with time, especially in the mixed Sn–Pb low-bandgap layer, limit performance and stability. Here, in this study, we find that mixed Sn–Pb perovskite thin films exhibit a compositional gradient, with an excess of Sn on the surface – and we show this gradient exacerbates oxidation and increases the recombination rate. We find that diamines preferentially chelate Sn atoms, removing them from the film surface and achieving a more balanced Sn:Pb stoichiometry, making the surface of the film resistive to the oxidation of Sn. The process forms an electrically resistive low-dimensional barrier layer, passivating defects and reducing interface recombination. Further improving the homogeneity of the barrier layer using 1,2-diaminopropane results in more uniform distribution and passivation. Tandems achieve a power conversion efficiency of 28.8%. As a result, encapsulated tandems retain 90% of initial efficiency following 1000 hours of operating at the maximum power point under simulated one-sun illumination in air without cooling.

14 SOLAR ENERGY↗

Generation of mean flows in rotating anisotropic turbulence: The case of solar near-surface shear layer

Results from helioseismology indicate that the radial gradient of the rotation rate in the near-surface shear layer (NSSL) of the Sun is independent of latitude and radius. Theoretical models using the mean-field approach have been successful in explaining this property of the NSSL, while global direct or large-eddy magnetoconvection models have so far been unable to reproduce this. We investigate the reason for this discrepancy by measuring the mean flows, Reynolds stress, and turbulent transport coefficients under conditions mimicking those in the solar NSSL. Simulations with as few ingredients as possible to generate mean flows were studied. These ingredients are inhomogeneity due to boundaries, anisotropic turbulence, and rotation. The parameters of the simulations were chosen such that they matched the weakly rotationally constrained NSSL. The simulations probe locally Cartesian patches of the star at a given depth and latitude. The depth of the patch was varied by changing the rotation rate such that the resulting Coriolis numbers covered the same range as in the NSSL. We measured the turbulent transport coefficient relevant for the nondiffusive (Λ-effect) and diffusive (turbulent viscosity) parts of the Reynolds stress and compared them with predictions of current mean-field theories. A negative radial gradient of the mean flow is generated only at the equator where meridional flows are absent. At other latitudes, the meridional flow is comparable to the mean flow corresponding to differential rotation. We also find that the meridional components of the Reynolds stress cannot be ignored. Additionally, we find that the turbulent viscosity is quenched by rotation by about 50% from the surface to the bottom of the NSSL. Our local simulations do not validate the explanation for the generation of the NSSL from mean-field theory where meridional flows and stresses are neglected. However, the rotational dependence of the turbulent viscosity in our simulations agrees well with theoretical predictions. Moreover, our results agree qualitatively with global convection simulations in that an NSSL can only be obtained near the equator.

79 ASTRONOMY AND ASTROPHYSICS↗

Closure to “Observation-Based Evaluation of Flood Estimation Techniques for a Small Snow-Dominated Basin in the Washington Cascade Mountains”

Here, this paper presents a closure to “Observation-Based Evaluation of Flood Estimation Techniques for a Small Snow-Dominated Basin in the Washington Cascade Mountains” by Hongxiang Yan, Zhuoran Duan, Mark S. Wigmosta, Ning Sun, Ethan D. Gutmann, Bert Kruyt, and Jeffrey R. Arnold. https://doi.org/10.1061/JHYEFF .HEENG-6147.

54 ENVIRONMENTAL SCIENCES↗

Enhancement of edge turbulence concomitant with ELM suppression during boron powder injection in EAST

A reproducible, quasi-stationary edge localized mode (ELM)-suppressed scenario was obtained over a wide range of plasma parameters by continuous injection of boron (B) powder into an upper-single null discharge in the experimental advanced superconducting tokamak [Sun et al., Nucl. Fusion 61, 014002 (2021)]. This powder-induced ELM-absent regime is associated with an edge harmonic mode (EHM) that provides continuous particle exhaust to maintain constant density without confinement degradation and impurity accumulation, the latter of which is often observed in ELM-free regimes. A flow rate threshold of B powder injection, leading to a threshold intensity of the EHM, is necessary for full ELM suppression. The fundamental harmonic of the EHM exhibits a toroidal mode number n = 1. The mode is observable in the entire poloidal cross section with a peak near the upper X-point in an upper-single null configuration. Here, the EHM spans radially across the pedestal and scrape-off layer, peaking inside the separatrix. The EHM appears to be insensitive to q 95 , heating power, plasma toroidal rotation, and pedestal collisionality.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Stability of superthermal strahl electrons in the solar wind

We present a kinetic stability analysis of the solar wind electron distribution function consisting of the Maxwellian core and the magnetic-field aligned strahl, a superthermal electron beam propagating away from the sun. We use an electron strahl distribution function obtained as a solution of a weakly collisional drift-kinetic equation, representative of a strahl affected by Coulomb collisions but unadulterated by possible broadening from turbulence. This distribution function is essentially non-Maxwellian and varies with the heliospheric distance. The stability analysis is performed with the Vlasov–Maxwell linear solver leopard. We find that depending on the heliospheric distance, the core-strahl electron distribution becomes unstable with respect to sunward-propagating kinetic-Alfvén, magnetosonic, and whistler modes, in a broad range of propagation angles. The wavenumbers of the unstable modes are close to the ion inertial scales, and the radial distances at which the instabilities first appear are on the order of 1 au. However, we have not detected any instabilities driven by resonant wave interactions with the superthermal strahl electrons. Instead, the observed instabilities are triggered by a relative drift between the electron and ion cores necessary to maintain zero electric current in the solar wind frame (ion frame). Contrary to strahl distributions modelled by shifted Maxwellians, the electron strahl obtained as a solution of the kinetic equation is stable. Our results are consistent with the previous studies based on a more restricted solution for the electron strahl.

79 ASTRONOMY AND ASTROPHYSICS↗

AlgoSCR: an algorithm for solar contamination removal from radio interferometric data

Hydrogen intensity mapping is a new field in astronomy that promises to make three-dimensional maps of the matter distribution of the Universe using the redshifted 21cm line of neutral hydrogen gas (HI). Several ongoing and upcoming radio interferometers, such as Tianlai, CHIME, HERA, HIRAX, etc., are using this technique. These instruments are designed to map large swaths of the sky by drift scanning over periods of many months. One of the challenges of the observations is that the daytime data are contaminated by strong radio signals from the Sun. In the case of Tianlai, this results in almost half of the measured data being unusable. We try to address this issue by developing an algorithm for solar contamination removal (AlgoSCR) from the radio data. The algorithm is based on an eigenvalue analysis of the visibility matrix and hence is applicable only to interferometers. We apply AlgoSCR to simulated visibilities, as well as real daytime data from the Tianlai dish array. The algorithm can reduce strong solar contamination by about 95 per cent without seriously affecting other weaker sky signals and thus makes the data usable for certain applications.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Seasonal changes in GPP/SIF ratios and their climatic determinants across the Northern Hemisphere

Satellite-derived sun-induced chlorophyll fluorescence (SIF) has been increasingly used for estimating gross primary production (GPP). However, the relationship between SIF and GPP has not been well defined, impeding the translation of satellite observed SIF to GPP. Previous studies have generally assumed a linear relationship between SIF and GPP at daily and longer time scales, but support for this assumption is lacking. Here, we used the GPP/SIF ratio to investigate seasonal variations in the relationship between SIF and GPP over the Northern Hemisphere (NH). Based on multiple SIF products and MODIS and FLUXCOM GPP data, we found strong seasonal hump-shaped patterns for the GPP/SIF ratio over northern latitudes, with higher values in the summer than in the spring or autumn. This hump-shaped GPP/SIF seasonal variation was confirmed by examining different SIF products and was evident for most vegetation types except evergreen broadleaf forests. The seasonal amplitude of the GPP/SIF ratio decreased from the boreal/arctic region to drylands and the tropics. For most of the NH, the lowest GPP/SIF values occurred in October or September, while the maximum GPP/SIF values were evident in June and July. The most pronounced seasonal amplitude of GPP/SIF occurred in intermediate temperature and precipitation ranges. GPP/SIF was positively related to temperature in the early and late parts of the growing season, but not during the peak growing months. These shifting relationships between temperature and GPP/SIF across different months appeared to play a key role in the seasonal dynamics of GPP/SIF. Several mechanisms may explain the patterns we observed, and future research encompassing a broad range of climate and vegetation settings is needed to improve our understanding of the spatial and temporal relationships between SIF and GPP. Nonetheless, the strong seasonal variation in GPP/SIF we identified highlights the importance of incorporating this behavior into SIF-based GPP estimations.

54 ENVIRONMENTAL SCIENCES↗

An exploratory steady–state redox model of photosynthetic linear electron transport for use in complete modelling of photosynthesis for broad applications

A photochemical model of photosynthetic electron transport (PET) is needed to integrate photophysics, photochemistry, and biochemistry to determine redox conditions of electron carriers and enzymes for plant stress assessment and mechanistically link sun-induced chlorophyll fluorescence to carbon assimilation for remotely sensing photosynthesis. Towards this goal, we derived photochemical equations governing the states and redox reactions of complexes and electron carriers along the PET chain. These equations allow the redox conditions of the mobile plastoquinone pool and the cytochrome b 6 f complex (Cyt) to be inferred with typical fluorometry. The equations agreed well with fluorometry measurements from diverse C 3 /C 4 species across environments in the relationship between the PET rate and fraction of open photosystem II reaction centres. We found the oxidation of plastoquinol by Cyt is the bottleneck of PET, and genetically improving the oxidation of plastoquinol by Cyt may enhance the efficiency of PET and photosynthesis across species. Redox reactions and photochemical and biochemical interactions are highly redundant in their complex controls of PET. Although individual reaction rate constants cannot be resolved, they appear in parameter groups which can be collectively inferred with fluorometry measurements for broad applications. The new photochemical model developed enables advances in different fronts of photosynthesis research.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

A rechargeable zinc-air battery based on zinc peroxide chemistry

When two is better than four Batteries based on the reaction of zinc and oxygen have been used for more than a century, but these have been primary (that is, nonrechargeable) cells. These batteries use an alkaline electrolyte and require a four-electron reduction of oxygen to water, which is a slow process. Sun et al. show that with the right choice of nonalkaline electrolyte, the battery can operate using a two-electron zinc-oxygen/zinc peroxide chemistry that is far more reversible. By making the electrolyte hydrophobic, water is excluded from the near surface of the cathode, thus preventing the four-electron reduction. These batteries also show higher energy density and better cycling stability. Science , this issue p. 46

Science & Technology - Other Topics↗