Temporal Dynamics and Performance Association of the Tetrasphaera-Enriched Microbiome for Enhanced Biological Phosphorus Removal

Tetrasphaera have been recently identified based on the 16S ribosomal RNA(rRNA)gene as among the most abundant polyphosphate-accumulating organisms(PAOs)in global full-scale wastewater treatment plants(WWTPs)with enhanced biological phosphorus removal(EBPR).However,it is unclear how Tetrasphaera PAOs are selectively enriched in the context of the EBPR microbiome.In this study,an EBPR microbiome enriched with Tetrasphaera(accounting for 40%of 16S sequences on day 113)was built using a top-down design approach featuring multicarbon sources and a low dosage of allylthiourea.The microbiome showed enhanced nutrient removal(phosphorus removal~85%and nitrogen removal~80%)and increased phosphorus recovery(up to 23.2 times)compared with the seeding activated sludge from a local full-scale WWTP.The supply of 1 mg·L^(-1)allylthiourea promoted the coselection of Tetrasphaera PAOs and Microlunatus PAOs and sharply reduced the relative abundance of both ammonia oxidizer Nitrosomonas and putative competitors Brevundimonas and Paracoccus,facilitating the establishment of the EBPR microbiome.Based on 16S rRNA gene analysis,a putative novel PAO species,EBPR-ASV0001,was identified with Tetrasphaera japonica as its closest relative.This study provides new knowledge on the establishment of a Tetrasphaera-enriched microbiome facilitated by allylthiourea,which can be further exploited to guide future process upgrading and optimization to achieve and/or enhance simultaneous biological phosphorus and nitrogen removal from high-strength wastewater.

A Generalized Polymer Precursor Ink Design for 3D Printing of Functional Metal Oxides

Three-dimensional-structured metal oxides have myriad applications for optoelectronic devices.Comparing to conventional lithography-based manufacturing methods which face significant challenges for 3D device architectures,additive manufacturing approaches such as direct ink writing offer convenient,on-demand manufacturing of 3D oxides with high resolutions down to sub-micrometer scales.However,the lack of a universal ink design strategy greatly limits the choices of printable oxides.Here,a universal,facile synthetic strategy is developed for direct ink writable polymer precursor inks based on metal-polymer coordination effect.Specifically,polyethyleneimine functionalized by ethylenediaminetetraacetic acid is employed as the polymer matrix for adsorbing targeted metal ions.Next,glucose is introduced as a crosslinker for endowing the polymer precursor inks with a thermosetting property required for 3D printing via the Maillard reaction.For demonstrations,binary(i.e.,ZnO,CuO,In_(2)O_(3),Ga_(2)O_(3),TiO_(2),and Y_(2)O_(3)) and ternary metal oxides(i.e.,BaTiO_(3) and SrTiO_(3)) are printed into 3D architectures with sub-micrometer resolution by extruding the inks through ultrafine nozzles.Upon thermal crosslinking and pyrolysis,the 3D microarchitectures with woodpile geometries exhibit strong light-matter coupling in the mid-infrared region.The design strategy for printable inks opens a new pathway toward 3D-printed optoelectronic devices based on functional oxides.

Chiral Betaine-Mediated Asymmetric Peroxidation-Kinetic Resolution Cascade for the Synthesis of Optically Pure Peroxides

An array of natural products bearing chiral peroxide motifs display antitumor,anticancer,and antiparasitic activities.However,there are very few catalytic asymmetric syntheses of chiral peroxides.Moreover,effective catalysts for asymmetric catalytic peroxidations are limited to chiral amines.To further expand synthetic access to chiral peroxides,the development of new catalysts realizing catalytic asymmetric peroxidation is highly desirable yet challenging.We report here a catalytic asymmetric peroxidation of anα,β-unsaturated triflone-kinetic resolution cascade reaction,which furnishes chiral peroxides in greater than 99.9%ee.The realization of this cascade reaction resulted from the development of two betaines as novel catalysts for chiral peroxide synthesis;one betaine promoted enantioselective peroxidation ofα,β-unsaturated triflones via conjugate addition affording peroxides in 80-92%ee,while the other betaine catalyzed kinetic resolution of the newly generated chiral peroxides to further increase the ee to greater than 99.9%.

Nutri-microbiome epidemiology,an emerging field to disentangle the interplay between nutrition and microbiome for human health

Diet and nutrition have a substantial impact on the human microbiome,and interact with the microbiome,especially gut microbiome,to modulate various diseases and health status.Microbiome research has also guided the nutrition field to a more integrative direction,becoming an essential component of the rising area of precision nutrition.In this review,we provide a broad insight into the interplay among diet,nutrition,microbiome,and microbial metabolites for their roles in the human health.Among the microbiome epidemiological studies regarding the associations of diet and nutrition with microbiome and its derived metabolites,we summarize those most reliable findings and highlight evidence for the relationships between diet and disease-associated microbiome and its functional readout.Then,the latest advances of the microbiome-based precision nutrition research and multidisciplinary integration are described.Finally,we discuss several outstanding challenges and opportunities in the field of nutri-microbiome epidemiology.

Recent advances in the synthesis and applications of furocoumarin derivatives

Furocoumarins are an important class of heterocyclic compounds with a fused tricyclic structure of coumarin and furan rings.They are commonly found in bioactive natural products and have a diverse range of biological and pharmaceutical properties,including cytotoxicity,photosensitivity,insecticidal,antibacterial,and antifungal activity,among others.The elegant linear/angular tricyclic skeleton and superior pharmacological properties,make them ideal for building and developing advanced biological scaffolds for biomedical applications.As a result,the family of furocoumarins has been the focus of intensive research,and lots of encouraging progress have been achieved in recent years.This review summarizes the most recent methods reported for the synthesis of the furocoumarin derivative family,along with their applications in medicinal chemistry covering from 2018 to 2022.

Multimaterial Embedded 3D Printing of Composite Reinforced Soft Actuators

Soft pneumatic actuators(SPAs)have attracted enormous attention in the growing field of robotics.Among different SPAs,composite reinforced actuators(CRAs)are widely used because of their simple structure and high controllability.However,multistep molding,a time-consuming method,is still the predominant fabrication method.Here,we propose a multimaterial embedded printing method(ME3P)to fabricate CRAs.In comparison with other 3-dimensional printing methods,our method improves fabrication flexibility greatly.Via the design and fabrication of the reinforced composites’patterns and different geometries of the soft body,we demonstrate actuators with programmable responses(elongation,contraction,twisting,bending,and helical and omnidirectional bending).Finite element analysis is employed for the prediction of pneumatic responses and the inverse design of actuators based on specific actuation needs.Lastly,we use tube-crawling robots as a model system to demonstrate our ability to fabricate complex soft robots for practical applications.This work demonstrates the versatility of ME3P for the future manufacturing of CRA-based soft robots.

Can the Super-deduction of R&D Expenses BoostR&DInvestment?

The super-deduction of research and development(R&D)expenses is at the core of the policy to stimulate enterprise innovation in China.This paper identifies whether firms are supported by the super-deduction policies for R&D expenses and uses the diferencein-diferences method to investigate the impact of the policies on R&D investment.The results show that changes in policy in 2013 significantly increased the R&D investment of firms engaging in key state-supported technologies.Policy changes in 2016 significantly increased the R&D investment of firms engaging in non-key-state-supported technologies.Enterprises not only invested all their tax incentives in R&D activities but also increased their investment in self-raised funds.The super-deduction policy had different impacts on different industries,firms with different boards,and firms with diferent ownership.The policy significantly affected the manufacturing and construction industries,the Small and Medium Enterprise Board,and non-state-owned enterprises.Through a mechanism analysis,we found that the policy significantly reduced the user cost of R&D and increased the net cash flow of enterprises,which could raise a firm's R&D investment.It is necessary to increase policy support,expand the scope of super-deductible expenses,and increase the super-deduction rate based on industry classification according to the sensitivity of different industries to the policy.

Rhodium-catalyzed addition reactions of benzylic C–H bonds to cyclic N-sulfonyl ketimines viaπ-coordination

Mannich-type reactions are a widely used method for the synthesis of amines due to the readily availability of nucleophiles and electrophiles.However,the inclusion of alkylarenes instead of active carbon pronucleophiles such as aldehydes and ketones in these addition reactions has been a challenge due to the inherent difficulty of benzylic deprotonation.In this study,we present a novel approach for the construction of N-sulfonyl amines via rhodium-catalyzed addition of unbiased benzylic C–H bonds to cyclic N-sulfonyl ketamines throughπ-coordination.This strategy enables the synthesis of a diverse range of N-sulfonyl amines,and subsequent diversification of the addition products showcases the synthetic potential of this protocol.

A distinction of gliomas at cellular and tissue level by surface-enhanced Raman scattering spectroscopy

Glioblastoma multiforme(GBM)is the most common malignant primary brain tumor in adults.The precise identification and distinction of GBM heterogeneity from surrounding brain parenchyma at the cellular level and even at the tissue level are important for GBM therapy.In this study,GBM cells are distinguished from normal astrocytes and non-central nervous system(CNS)tumor cells by surface-enhanced Raman scattering(SERS)based on gold nanoshell(SiO_(2)@Au)particles and support vector machine(SVM)algorithm.In addition,the gold nanoisland(AuNI)SERS substrates are further developed and explored for accurate detection of GBM at the tissue level.The distinction between glioma and trauma tissues,identification of different tumor grades,and IDH mutation are realized with the assistance of orthogonal partial least squares discriminant analysis(OPLS-DA)in a rapid,non-invasive,and convenient method.The results show that the developed SERS-based analytical method has the potential for practical application for the detection of GBM at the single-cell and tissue levels and even for real-time intraoperative diagnosis.

Modulation of polymerization rate of N-carboxyanhydrides in a biphasic system

The recent advances in accelerated polymerization of N-carboxyanhydrides (NCAs) offer an effective strategy to simplify the preparation of polypeptide materials. However, the fine-tuning of polymerization kinetics, which is critical to differentiate the main polymerization and the side reactions, remains largely unexplored. Herein we report the modulation of polymerization rate of NCA in a water/oil biphasic system. By altering the aqueous pH, the initial location of the initiators, and the pK_(a) of initiating amines, we observed the change in polymerization time from several minutes to a few hours. Due to the high interfacial activity and low pKa value, controlled polymerization was observed from multi-amine initiators even if they were initially located in the aqueous phase. This work not only improves our understanding on the biphasic polymerization mechanism, but also facilitates preparation of versatile polypeptide materials.

Installing hydrogen bonds as a general strategy to control viscosity sensitivity of molecular rotor fluorophores Special Collection:Aggregation-Induced Processes and Functions

Molecular rotor-based fluorophores(RBFs)activate fluorescence upon increase of micro-viscosity,thus bearing a broad application promise in many fields.However,it remains a challenge to control how fluorescence of RBFs responds to viscosity changes.Herein,we demonstrate that the formation and regulation of intramolecular hydrogen bonds in the excited state of RBFs could modulate their rotational barrier,leading to a rational control of how their fluorescence can be activated by micro-viscosity.Based on this strategy,a series of RBFs were developed based on 4-hydroxybenzylidene-imidazolinone(HBI)that span a wide range of viscosity sensitivity.Combined with the AggTag method that we previously reported,the varying viscosity sensitivity and emission spectra of these probes enabled a dualcolor imaging strategy that detects both protein oligomers and aggregates during the multistep aggregation process of proteins in live cells.In summary,our work indicates that installing intracellular excited state hydrogen bonds to RBFs allows for a rational control of rotational barrier,thus allow for a fine tune of their viscosity sensitivity.Beyond RBFs,we envision similar strategies can be applied to control the fluorogenic behavior of a large group of fluorophores whose emission is dependent on excited state rotational motion,including aggregation-induced emission fluorophores.

Fight or flee,a vital choice for Clostridioides difficile

Clostridioides difficile is a leading cause of healthcare-associated infections,causing billions of economic losses every year.Its symptoms range from mild diarrhea to life-threatening damage to the colon.Transmission and recurrence of c.difficile infection(CDl)are mediated by the metabolically dormant spores,while the virulence of C.difficile is mainly due to the two large clostridial toxins,TcdA and TcdB.Producing toxins or forming spores are two different strategies for C.difficile to cope with harsh environmental conditions.It is of great significance to understand the molecular mechanisms for C.difficile to skew to either of the cellular processes.Here,we summarize the current understanding of the regulation and connections between toxin production and sporulation in C.difficile and further discuss the potential solutions for yet-to-be-answered questions.

Roadmap for rechargeable batteries:present and beyond

Rechargeable batteries currently hold the largest share of the electrochemical energy storage market,and they play a major role in the sustainable energy transition and industrial decarbonization to respond to global climate change.Due to the increased popularity of consumer electronics and electric vehicles,lithium-ion batteries have quickly become the most successful rechargeable batteries in the past three decades,yet growing demands in diversified application scenarios call for new types of rechargeable batteries.Tremendous efforts are made to developing the next-generation post-Li-ion rechargeable batteries,which include,but are not limited to solid-state batteries,lithium–sulfur batteries,sodium-/potassium-ion batteries,organic batteries,magnesium-/zinc-ion batteries,aqueous batteries and flow batteries.Despite the great achievements,challenges persist in precise understandings about the electrochemical reaction and charge transfer process,and optimal design of key materials and interfaces in a battery.This roadmap tends to provide an overview about the current research progress,key challenges and future prospects of various types of rechargeable batteries.New computational methods for materials development,and characterization techniques will also be discussed as they play an important role in battery research.

A dual-functional BODIPY-based molecular rotor probe reveals different viscosity of protein aggregates in live cells

Aberrant protein aggregation leads to various human diseases,but little is known about the physical chemical properties of these aggregated proteins in cells.Herein,we developed a boron-dipyrromethene(BODIPY)-based HaloTag probe,whose conjugation to HaloTag-fused proteins allows us to study protein aggregates using both fluorescence intensity and lifetime.Modulation of BODIPY fluorophore reveals key structural features to attain the dual function.The optimized probe exhibits increased fluorescence intensity and elongated fluorescence lifetime in protein aggregates.Fluorescence lifetime imaging using this probe indicates that protein aggregates afford different viscosity in the forms of soluble oligomers and insoluble aggregates in live cells.The strategy presented in this work can be extended to enable a wide class of HaloTag probes that can be used to study a variety of physical properties of protein aggregates,thus helping unravel the pathogenic mechanism and develop therapeutic strategy.

From atomistic modeling to materials design:computation-driven material development in lithium-ion batteries

As an advanced energy storage system,lithium-ion batteries play an essential role in modern technologies.Despite their ubiquitous success,there is a great demand for continuous improvements of the battery performance,including higher energy density,lower safety risk,longer cycling life,and lower cost.Such performance improvement requires the design and development of novel electrode and electrolyte materials that exhibit desirable properties and satisfy strict requirements.Atomistic modeling can provide a unique perspective to fundamentally understand and rationally design battery materials.In this paper,we review a few recent successful examples of computation-driven discovery and design in electrode and electrolyte materials.Particularly,we highlight how atomistic modeling can reveal the underlying mechanisms,predict the important properties,and guide the design and engineering of electrode and electrolyte materials.We have a conclusion with a discussion of the unique capability of atomistic modeling in battery material development and provide a perspective on future challenges and directions for computation-driven battery material developments.

Cr-catalyzed allylic C(sp~3)–H addition to aldehydes enabled by photoinduced ligand-to-metal charge transfer

Photoinduced ligand-to-metal charge transfer(LMCT) has emerged as an effective strategy for synthesizing organic molecules in a sustainable manner. However, the majority of existing reports on selective C(sp~3)–H bond functionalization via photoinduced LMCT focus on the use of late transition metals or rare-earth metals for radical additions or cross-couplings. In contrast, the utilization of photoinduced LMCT with 3d early transition metals poses a significant challenge. Herein, we describe an unprecedented approach to allylic C(sp~3)–H addition to aldehydes, employing chromium(Cr) complexes as catalysts through visible-light-induced LMCT. By investigating the reaction pathway through various mechanistic studies, including radical trapping, kinetic isotope effect(KIE) analysis, and transient absorption spectroscopy, valuable insights have been gained. The proposed mechanism suggests the intermediacy of bromine radicals through homolysis of the Cr–Br bond. Notably, this protocol expands our understanding of the photochemical properties of earth-abundant Cr complexes.

Snapshot spectral compressive imaging reconstruction using convolution and contextual Transformer

Spectral compressive imaging(SCI) is able to encode a high-dimensional hyperspectral image into a twodimensional snapshot measurement, and then use algorithms to reconstruct the spatio-spectral data-cube. At present, the main bottleneck of SCI is the reconstruction algorithm, and state-of-the-art(SOTA) reconstruction methods generally face problems of long reconstruction times and/or poor detail recovery. In this paper, we propose a hybrid network module, namely, a convolution and contextual Transformer(CCo T) block, that can simultaneously acquire the inductive bias ability of convolution and the powerful modeling ability of Transformer, which is conducive to improving the quality of reconstruction to restore fine details. We integrate the proposed CCo T block into a physics-driven deep unfolding framework based on the generalized alternating projection(GAP) algorithm, and further propose the GAP-CCo T network. Finally, we apply the GAP-CCo T algorithm to SCI reconstruction. Through experiments on a large amount of synthetic data and real data,our proposed model achieves higher reconstruction quality(>2 d B in peak signal-to-noise ratio on simulated benchmark datasets) and a shorter running time than existing SOTA algorithms by a large margin. The code and models are publicly available at https://github.com/ucaswangls/GAP-CCoT.

Developing Classical Interatomic Potentials for Solid Electrolytes

All-solid-state battery is one of the most promising candidates for the next stage of energy storage systems.With improved safety,increased energy density,longer cycling life,and higher power density,all-solid-state battery is considered as a potential successor and complement to the currently commercialized lithium-ion battery.A key compo-nent of all-solid-state lithium-ion battery includes the solid electrolyte materials,which are ceramic-based lithium superi-onic conductors.Ideal solid electrolyte materials should have high ionic conductivity(>1 mS/cm)at room temperature,which is a rare property for most lithium-containing inorganic materials.

High-sensitive two-dimensional PbI_(2)photodetector with ultrashort channel

Photodetectors based on two-dimensional(2D)semiconductors have attracted many research interests owing to their excellent optoelectronic characteristics and application potential for highly integrated applications.However,the unique morphology of 2D materials also restricts the further improvement of the device performance,as the carrier transport is very susceptible to intrinsic and extrinsic environment of the materials.Here,we report the highest responsivity(172 A/W)achieved so far for a PbI_(2)-based photodetector at room temperature,which is an order of magnitude higher than previously reported.Thermal scanning probe lithography(t-SPL)was used to pattern electrodes to realize the ultrashort channel(~60 nm)in the devices.The shortening of the channel length greatly reduces the probability of the photo-generated carriers being scattered during the transport process,which increases the photocurrent density and thus the responsivity.Our work shows that the combination of emerging processing technologies and 2D materials is an effective route to shrink device size and improve device performance.

Shift current response in elemental two-dimensional ferroelectrics

A bulk material without inversion symmetry can generate a direct current under illumination.This interface-free current generation mechanism,referred to as the bulk photovoltaic effect(BPVE),does not rely on p-n junctions.Here,we explore the shift current generation,a major mechanism responsible for the BPVE,in single-element two-dimensional(2D)ferroelectrics represented by phosphorene-like monolayers of As,Sb,and Bi.The strong covalency,small band gap,and large joint density of states afforded by these elemental 2D materials give rise to large shift currents,outperforming many state-of-the-art materials.We find that the shift current,due to its topological nature,depends sensitively on the details of the Bloch wave functions.It is crucial to consider the electronic exchange-correlation potential beyond the generalized gradient approximation as well as the spin-orbit interaction in density functional theory calculations to obtain reliable frequency-dependent shift current responses.