Yuting LiangHan HuThomas W.CrowtherRainer Georg Jörgensen...
104-110页
查看更多>>摘要：Soil organic carbon(SOC)represents the largest terrestrial pool of organic carbon and is indispensable for mitigating climate change and sustaining soil fertility.As a major component of stable SOC,microbial-derived carbon(MDC)accounts for approximately half of the total SOC and has repercussions on climate feedback.However,our understanding of the spatial and temporal dynamics of MDC stocks is limited,hindering assessments of the long-term impacts of global warming on persistent SOC sequestration in the soil-atmosphere carbon cycle.Here,we compiled an extensive global dataset and employed ensemble machine learning techniques to forecast the spatial-temporal dynamics of MDC stocks across 93.4％of the total global land area from 1981 to 2018.Our findings revealed that for every 1℃ increase in temperature,there was a global decrease of 6.7 Pg in the soil MDC stock within the predictable areas,equivalent to 1.4％of the total MDC stock or 0.9％of the atmospheric C pool.Tropical regions experienced the most substantial declines in MDC stocks.We further projected future MDC stocks for the next century based on shared socioeconomic pathways,showing a global decline in MDC stocks with a potential 6-37 Pg reduction by 2100 depending on future pathways.We recommend integrating the response of MDC stocks to warming into socioeconomic models to enhance confidence in selecting sustainable pathways.
查看更多>>摘要：Ozone pollution is a major environmental threat to human health.Timely assessment of ozone trends is crucial for informing environmental policy.Here we show that for the most recent decade(2013-2022)in the northern hemisphere,warm-season(April-September)mean daily 8-h average maximum ozone increases much faster in urban regions with top ozone levels(mainly in the North China Plain,1.2±1.3 ppbv year-1)than in other,low-ozone regions(0.2±0.9 ppbv year-1).These trends widen the ozone differences across urban regions,and increase extreme pollution levels and health threats from a global perspective.Comparison of historical trends in different urban regions reveals that ozone increases in China during 2013-2022 differ in magnitude and mechanisms to historical periods in other regions since 1980.This reflects a unique chemical environment characterized by exceptionally high nitrogen oxides and aerosol concentrations,where reducing ozone precursor emissions leads to substantial ozone increase.Ozone increase in China has slowed down in 2018-2022 compared to 2013-2017,driven by ongoing emission reductions,but with ozone-favorable weather conditions.Historical ozone evolution in Japan and South Korea indicates that ozone increases should be suppressed with continuous emission reduction.Increasing temperature and associated wildfires have also reversed ozone decreases in the USA and Europe,with anthropogenic ozone control slowing down in recent decades.
查看更多>>摘要：The development of alternative methods to the Haber-Bosch process for ammonia(NH3)synthesis is a pressing and formidable challenge.Nuclear energy represents a low-carbon,efficient and stable source of power.The harnessing of nuclear energy to drive nitrogen(N2)reduction not only allows'green'NH3 synthesis,but also offers the potential for the storage of nuclear energy as a readily transportable zero-carbon fuel.Herein,we explore radiocatalytic N2 fixation to NH3 induced by γ-ray radiation.Hydrated electrons(e-aq)that are generated from water radiolysis enable N2 reduction to produce NH3.Ru-based catalysts synthesized by using γ-ray radiation with excellent radiation stability substantially improve NH3 production in which the B5 sites of Ru particles may play an important role in the activation of N2.By benefitting from the remarkable penetrating power of γ-ray radiation,radiocatalytic NH3 synthesis can proceed in an autoclave under appropriate pressure conditions,resulting in an NH3 concentration of≤5.1 mM.The energy conversion efficiency of the reaction is as high as 563.7 mgNH3.MJ-1.This radiocatalytic chemistry broadens the research scope of catalytic N2 fixation while offering promising opportunities for converting nuclear energy into chemical energy.
查看更多>>摘要：The direct epoxidation of propylene with molecular oxygen represents a desired route for propylene oxide(PO)production with 100％theoretical atomic economy.However,this aerobic epoxidation reaction suffers from the apparent trade-off between propylene conversion and PO selectivity,and remains a key challenge in catalysis.We report that Ti-Beta zeolites containing isolated framework Ti species can efficiently catalyze the aerobic epoxidation of propylene.Stable propylene conversion of 25％and PO selectivity of up to 90％are achieved at the same time,matching the levels of industrial ethylene aerobic epoxidation processes.H-terminated pentacoordinated Ti species in Beta zeolite frameworks are identified as the preferred active sites for propylene aerobic epoxidation and the reaction is initiated by the participation of lattice oxygen in Ti-OH.These results are expected to spark new technology for the industrial production of PO toward more sustainable chemistry and chemical engineering.
查看更多>>摘要：Protein glycosylation,the most universal post-translational modification,is thought to play a crucial role in regulating multiple essential cellular processes.However,the low abundance of glycoproteins and the heterogeneity of glycans complicate their comprehensive analysis.Here,we develop a rapid and large-scale glycopeptide enrichment strategy via bioorthogonal ligation and trypsin cleavage.The enrichment process is performed in one tube to minimize sample loss and time costs.This method combines convenience and practicality,identifying over 900 O-GlcNAc sites from a 500 μg sample.Surprisingly,it allows simultaneous identification of N-glycosites,O-GlcNAc sites,O-GaINAc sites and N-glycans via a two-step enzymatic release strategy.Combined with quantitative analysis,it reveals the distinct O-GlcNAcylation patterns in different compartments during oxidative stress.In summary,our study offers a convenient and robust tool for glycoproteome and glycome profiling,facilitating in-depth analysis to elucidate the biological functions of glycosylation.
查看更多>>摘要：Abnormal levels of zinc ions within endo-lysosomes have been implicated in the progression of Alzheimer's disease(AD),yet the detection of low-concentration zinc ions at the organelle level remains challenging.Here we report the design of an endo-lysosome-targeted fluorescent reporter,Znluoriy,for imaging endogenous zinc ions.Znluoriy is constructed from an amphiphilic DNA framework(DNF)with programmable size and shape,which can encapsulate zinc-responsive fluorophores within its hydrophobic nanocavity.We find that the tetrahedral DNFs of 20 bp in the edge length are effectively located within endo-lysosomes,which can detect zinc ions with a detection limit of～31.9 nM(a sensitivity that is～2.5 times that of the free fluorophore).Given the organelle-targeting ability and high zinc sensitivity of Znluorly,we employ it to detect endogenous endo-lysosomal zinc ions in neuron cells.We monitor the dynamics of zinc levels in AD model cells and zebrafish,corroborating the positive correlation between zinc levels and AD hallmarks including Aβ aggregates and learning/memory impairments.Our study provides a generalizable strategy for organelle-specific theranostic applications.
查看更多>>摘要：The poor oxidation resistance of traditional electrolytes has hampered the development of high-voltage potassium-ion battery technology.Here,we present a cosolvent electrolyte design strategy to overcome the high-voltage limitations of potassium-ion electrolyte chemistries.The cosolvent electrolyte breaks the dissolution limitation of the salt through ion-dipole interactions,significantly enlarging the anion-rich solvation clusters,as verified by the in situ synchrotron-based wide-angle X-ray scattering experiments.Furthermore,the large anion-rich solvation clusters also facilitate the formation of an effective electrode-electrolyte interphase,thereby enhancing compatibility with high-voltage electrodes.The cosolvent electrolyte enables K‖ Prussian blue cells(2-4.5 V)to operate for＞700 cycles with a capacity retention of 91.9％.Our cosolvent electrolyte design strategy paves new avenues for the development of high-voltage potassium-ion batteries and beyond.
查看更多>>摘要：Implanted pressure sensors can provide pressure information to assess localized health conditions of specific tissues or organs,such as the intra-articular pressure within knee joints.However,the prerequisites for implanted sensors pose greater challenges than those for wearables or for robots:aside from biocompatibility and tissue-like softness,they must also exhibit humidity insensitivity and high-pressure resolution across a broad pressure spectrum.Iontronic sensors can provide superior sensing properties,but they undergo property degradation in wet environments due to the hygroscopic nature of their active component:ionogels.Herein,we introduce a humidity-insensitive iontronic sensor array based on a hydrophobic and tough ionogel polymerized in a hydrophobicity transition yielding two hydrophobic phases:a soft liquid-rich phase that enhances ionic conductivity and ductility,and a stiff polymer-rich phase that contributes to superior toughness.We demonstrate the in vivo implantation of these sensor arrays to monitor real-time intra-articular pressure distribution in a sheep model,while assessing knee flexion with an angular resolution of 0.1° and a pressure resolution of 0.1％.We anticipate that this sensor array will find applications in various orthopedic surgeries and implantable medical devices.
查看更多>>摘要：Epitaxy is the cornerstone of semiconductor technology,enabling the fabrication of single-crystal film.Recent advancements in van der Waals(vdW)epitaxy have opened new avenues for producing wafer-scale single-crystal 2D atomic crystals.However,when it comes to molecular crystals,the overall weak vdW force means that it is a significant challenge for small molecules to form a well-ordered structure during epitaxy.Here we demonstrate that the vdW epitaxy of Sb2O3 molecular crystal,where the whole growth process is governed by vdW interactions,can be precisely controlled.The nucleation is deterministically modulated by epilayer-substrate interactions and unidirectional nuclei are realized through designing the lattice and symmetry matching between epilayer and substrate.Moreover,the growth and coalescence of nuclei as well as the layer-by-layer growth mode are kinetically realized via tackling the Schwoebel-Ehrlich barrier.Such precise control of vdW epitaxy enables the growth of single-crystal Sb2O3 molecular film with desirable thickness.Using the ultrathin highly oriented Sb2O3 film as a gate dielectric,we fabricated MoS2-based field-effect transistors that exhibit superior device performance.The results substantiate the viability of precisely managing molecule alignment in vdW epitaxy,paving the way for large-scale synthesis of single-crystal 2D molecular crystals.
查看更多>>摘要：Bio-based aerogels,which are poised as compelling thermal insulators,demand intricate synthesis procedures and have limited durability under harsh conditions.The integration of smart stimuli-response transitions in biomass aerogels holds promise as a solution,yet remains a challenge.Here,we introduce a pioneering strategy that employs reversible-gel-assisted ambient-pressure drying without organic solvents to craft multifunctional bio-based aerogels.By exploiting the thermally reversible gelling propensity of select biomasses,we anchor emulsified bubbles within cross-linked hydrogels,circumventing surface tension issues during mild drying.The resultant aerogels feature a robust porous matrix that is imbued with stable bubbles,yielding low thermal conductivity,high flame retardancy and robust resistance to diverse rigors.This innovative approach facilitates a paradigm shift in intelligent fire protection in which aerogels transition from robust to flexible in response to water stimuli,effectively shielding against thermal hazards and external forces.This work opens up a facile,eco-friendly and mild way to fabricate advanced biomass aerogels with stimuli-responsive transformation.
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