Simultaneously quantifying hundreds of acylcarnitines in multiple biological matrices within ten minutes using ultrahigh-performance liquid-chromatography and tandem mass spectrometry

Acylcarnitines are metabolic intermediates of fatty acids and branched-chain amino acids having vital biofunctions and pathophysiological significances. Here, we developed a high-throughput method for quantifying hundreds of acylcarnitines in one run using ultrahigh performance liquid chromatography and tandem mass spectrometry (UPLC-MS/MS). This enabled simultaneous quantification of 1136 acylcarnitines (C0–C26) within 10-min with good sensitivity (limit of detection < 0.7 fmol), linearity (correlation coefficient > 0.992), accuracy (relative error < 20%), precision (coefficient of variation (CV), CV < 15%), stability (CV < 15%), and inter-technician consistency (CV < 20%, n = 6). We also established a quantitative structure-retention relationship (goodness of fit > 0.998) for predicting retention time (tR) of acylcarnitines with no standards and built a database of their multiple reaction monitoring parameters (tR, ion-pairs, and collision energy). Furthermore, we quantified 514 acylcarnitines in human plasma and urine, mouse kidney, liver, heart, lung, and muscle. This provides a rapid method for quantifying acylcarnitines in multiple biological matrices.

Personal Thermal Management by Radiative Cooling and Heating

Maintaining thermal comfort within the human body is crucial for optimal health and overall well-being.By merely broadening the setpoint of indoor temperatures,we could significantly slash energy usage in building heating,ventilation,and air-conditioning systems.In recent years,there has been a surge in advancements in personal thermal management(PTM),aiming to regulate heat and moisture transfer within our immediate surroundings,clothing,and skin.The advent of PTM is driven by the rapid development in nano/micro-materials and energy science and engineering.An emerging research area in PTM is personal radiative thermal management(PRTM),which demonstrates immense potential with its high radiative heat transfer efficiency and ease of regulation.However,it is less taken into account in traditional textiles,and there currently lies a gap in our knowledge and understanding of PRTM.In this review,we aim to present a thorough analysis of advanced textile materials and technologies for PRTM.Specifically,we will introduce and discuss the underlying radiation heat transfer mechanisms,fabrication methods of textiles,and various indoor/outdoor applications in light of their different regulation functionalities,including radiative cooling,radiative heating,and dual-mode thermoregulation.Furthermore,we will shine a light on the current hurdles,propose potential strategies,and delve into future technology trends for PRTM with an emphasis on functionalities and applications.

Toward understanding the role of genomic repeat elements in neurodegenerative diseases

Neurodegenerative diseases cause great medical and economic burdens for both patients and society;however, the complex molecular mechanisms thereof are not yet well understood. With the development of high-coverage sequencing technology, researchers have started to notice that genomic repeat regions, previously neglected in search of disease culprits, are active contributors to multiple neurodegenerative diseases. In this review, we describe the association between repeat element variants and multiple degenerative diseases through genome-wide association studies and targeted sequencing. We discuss the identification of disease-relevant repeat element variants, further powered by the advancement of long-read sequencing technologies and their related tools, and summarize recent findings in the molecular mechanisms of repeat element variants in brain degeneration, such as those causing transcriptional silencing or RNA-mediated gain of toxic function. Furthermore, we describe how in silico predictions using innovative computational models, such as deep learning language models, could enhance and accelerate our understanding of the functional impact of repeat element variants. Finally, we discuss future directions to advance current findings for a better understanding of neurodegenerative diseases and the clinical applications of genomic repeat elements.

Finding Ordered State in a Disordered Jungle

A rich portfolio of emergent phenomena has been discovered in twisted two-dimensional(2D)moirésystems,including strongly correlated insulators,[1]superconductivity,[2]integer and fractional Chern insulators(ChIs),[3-5]magnetism,[6]and interfacial ferroelectricity.

Lignin‐derived carbon with pyridine N‐B doping and a nanosandwich structure for high and stable lithium storage

Biomass‐derived carbon is a promising electrode material in energy storage devices.However,how to improve its low capacity and stability,and slow diffusion kinetics during lithium storage remains a challenge.In this research,we propose a“self‐assembly‐template”method to prepare B,N codoped porous carbon(BN‐C)with a nanosandwich structure and abundant pyridinic N‐B species.The nanosandwich structure can increase powder density and cycle stability by constructing a stable solid electrolyte interphase film,shortening the Li^(+)diffusion pathway,and accommodating volume expansion during repeated charging/discharging.The abundant pyridinic N‐B species can simultaneously promote the adsorption/desorption of Li^(+)/PF_(6)^(−)and reduce the diffusion barrier.The BN‐C electrode showed a high lithium‐ion storage capacity of above 1140 mAh g^(−1)at 0.05 A g^(−1)and superior stability(96.5%retained after 2000 cycles).Moreover,owing to the synergistic effect of the nanosandwich structure and pyridinic N‐B species,the assembled symmetrical BN‐C//BN‐C full cell shows a high energy density of 234.7Wh kg^(−1),high power density of 39.38 kW kg−1,and excellent cycling stability,superior to most of the other cells reported in the literature.As the density functional theory simulation demonstrated,pyridinic N‐B shows enhanced adsorption activity for Li^(+)and PF_(6)^(−),which promotes an increase in the capacity of the anode and cathode,respectively.Meanwhile,the relatively lower diffusion barrier of pyridinic N‐B promotes Li^(+)migration,resulting in good rate performance.Therefore,this study provides a new approach for the synergistic modulation of a nanostructure and an active site simultaneously to fabricate the carbon electrode material in energy storage devices.

Facet Engineering of Advanced Electrocatalysts Toward Hydrogen/Oxygen Evolution Reactions

The electrocatalytic water splitting technology can generate highpurity hydrogen without emitting carbon dioxide,which is in favor of relieving environmental pollution and energy crisis and achieving carbon neutrality.Electrocatalysts can effectively reduce the reaction energy barrier and increase the reaction efficiency.Facet engineering is considered as a promising strategy in controlling the ratio of desired crystal planes on the surface.Owing to the anisotropy,crystal planes with different orientations usually feature facet-dependent physical and chemical properties,leading to differences in the adsorption energies of oxygen or hydrogen intermediates,and thus exhibit varied electrocatalytic activity toward hydrogen evolution reaction(HER)and oxygen evolution reaction(OER).In this review,a brief introduction of the basic concepts,fundamental understanding of the reaction mechanisms as well as key evaluating parameters for both HER and OER are provided.The formation mechanisms of the crystal facets are comprehensively overviewed aiming to give scientific theory guides to realize dominant crystal planes.Subsequently,three strategies of selective capping agent,selective etching agent,and coordination modulation to tune crystal planes are comprehensively summarized.Then,we present an overview of significant contributions of facet-engineered catalysts toward HER,OER,and overall water splitting.In particular,we highlight that density functional theory calculations play an indispensable role in unveiling the structure–activity correlation between the crystal plane and catalytic activity.Finally,the remaining challenges in facet-engineered catalysts for HER and OER are provided and future prospects for designing advanced facet-engineered electrocatalysts are discussed.

Porous heterostructure of graphene/hexagonal boron nitride as an efficient electrocatalyst for hydrogen peroxide generation

Compared with the traditional heteroatom doping,employing heterostructure is a new modulating approach for carbon-based electrocatalysts.Herein,a facile ball milling-assisted route is proposed to synthesize porous carbon materials composed of abundant graphene/hexagonal boron nitride(G/h-BN)heterostructures.Metal Ni powder and nanoscale h-BN sheets are used as a catalytic substrate/hard template and“nucleation seed”for the formation of the heterostructure,respectively.As-prepared G/h-BN heterostructures exhibit enhanced electrocatalytic activity toward H_(2)O_(2) generation with 86%-95%selectivity at the range of 0.45-0.75 V versus reversible hydrogen electrode(RHE)and a positive onset potential of 0.79 versus RHE(defined at a ring current density of 0.3 mA cm^(-2))in the alkaline solution.In a flow cell,G/h-BN heterostructured electrocatalyst has a H_(2)O_(2) production rate of up to 762 mmol g_(catalyst)^(-1) h^(-1) and Faradaic efficiency of over 75%during 12 h testing,superior to the reported carbon-based electrocatalysts.The density functional theory simulation suggests that the B atoms at the interface of the G/h-BN heterostructure are the key active sites.This research provides a new route to activate carbon catalysts toward highly active and selective O_(2)-to-H_(2)O_(2) conversion.

Co@CoO:An efficient catalyst for the depolymerization and upgrading of lignocellulose to alkylcyclohexanols with cellulose intact

The depolymerization and upgrading of lignin from raw biomass,while keeping cellulose intact is important in biorefinery and various metal-based catalysts have been used in reductive catalytic fractionation,a key method in"lignin-first"strategy,Recently,we found that a core-shell structured Co@CoO catalyst with CoO shell as the real active site had excellent performance in the hydrogenolysis of 5-hydromethylfurfural to 2,5-dimethylfuran due to its unique ability to dissociate H_(2)and yield active H^(δ-)species(Xiang et al.,2022).In this work,we report a one-pot depolymerization and upgrading of lignocellulose to alkylcyclohexanols,a flavour precursor,with intact cellulose over this unique core-shell structured catalyst,Co@CoO.Lignin model compounds(β-O-4,4-O-5,α-O-4)were first used to clarify the activity of Co@CoO catalyst.Then,the one-pot conversion of various organosolv lignin(birch,pine and poplar)to alkylcyclohexanols was realized with the mass yield of alkylcyclohexanols up to25.8 wt%from birch lignin under the reaction condition of 210℃,1 MPa H_(2),16 h.Finally,the corresponding woody sawdusts were used as feedstocks and found that the Co@CoO catalyst indeed preferentially depolymerized and upgraded the lignin part and obtained the same alkylcyclohexanols products with the retention of cellulose-rich pulp.The collected alkylcyclohexanols were further esterified to obtain valueadded esters,which can be used as flavors.This work will inspire the design of new efficient metal oxide catalysts in lignin fractionation and depolymerization to high-value-added chemicals with intact cellulose.

Achieving highly selective electrochemical CO_(2) reduction to C_(2)H_(4) on Cu nanosheets

The conversion of CO_(2)into value-added chemicals coupled with the storage of intermittent renewable electricity is attractive.CuO nanosheets with an average size and thickness of~30 and~20 nm have been developed,which are in situ reduced into Cu nanosheets during electrochemical CO_(2)reduction reaction(ECO_(2)RR).The derived Cu nanosheets demonstrate much higher selectivity for C2H4production than commercial CuO derived Cu powder,with an optimum Faradaic efficiency of 56.2%and a partial current density of C_(2)H_(4)as large as 171.0 mA cm^(-2)in a gas diffusion flow cell.The operando attenuated total reflectance-Fourier transform infrared spectra measurements and density functional theory simulations illustrate that the high activity and selectivity of Cu nanosheets originate from the edge sites on Cu nanosheets with a coordinate number around 5(4–6),which facilitates the formation of^(*)CHO rather than^(*)COH intermediate,meanwhile boosting the C-C coupling reaction of^(*)CO and^(*)CHO intermediates,which are the critical steps for C_(2)H_(4)formation.

Catalytic conversion of lignocellulosic biomass into chemicals and fuels

In the search of alternative resources to make commodity chemicals and transportation fuels for a low carbon future,lignocellulosic biomass with over 180-billion-ton annual production rate has been identified as a promising feedstock.This review focuses on the state-of-the-art catalytic transformation of lignocellulosic biomass into value-added chemicals and fuels.Following a brief introduction on the structure,major resources and pretreatment methods of lignocellulosic biomass,the catalytic conversion of three main components,i.e.,cellulose,hemicellulose and lignin,into various compounds are comprehensively discussed.Either in separate steps or in one-pot,cellulose and hemicellulose are hydrolyzed into sugars and upgraded into oxygen-containing chemicals such as 5-HMF,furfural,polyols,and organic acids,or even nitrogen-containing chemicals such as amino acids.On the other hand,lignin is first depolymerized into phenols,catechols,guaiacols,aldehydes and ketones,and then further transformed into hydrocarbon fuels,bioplastic precursors and bioactive compounds.The review then introduces the transformations of whole biomass via catalytic gasification,catalytic pyrolysis,as well as emerging strategies.Finally,opportunities,challenges and prospective of woody biomass valorization are highlighted.

Two-Dimensional Thermal Regulation Based on Non-Hermitian Skin Effect

The non-Hermitian skin effect has been applied in multiple fields.However,there are relatively few models in the field of thermal diffusion that utilize the non-Hermitian skin effect for achieving thermal regulation.Here,we propose two non-Hermitian Su-Schrieffer-Heeger(SSH)models for thermal regulation:one capable of achieving edge states,and the other capable of achieving corner states within the thermal field.By analyzing the energy band structures and the generalized Brillouin zone,we predict the appearance of the non-Hermitian skin effect in these two models.Furthermore,we analyze the time-dependent evolution results and assess the robustness of the models.The results indicate that the localized thermal effects of the models align with our predictions.In a word,this work presents two models based on the non-Hermitian skin effect for regulating the thermal field,injecting vitality into the design of non-Hermitian thermal diffusion systems.

The case-dependent lignin role in lignocellulose nanofibers preparation and functional application-A review

Lignocellulose nanofibers(LCNFs) as a new material is attracting extensive attention. The pretreatment and mechanical fibrillation are the two main stages involved in the preparation of LCNFs, and lignin plays the important role of these two stages. This review discussed the interaction between lignin and chemicals in the pretreatment stage, and discovered the general law of the effect of lignin in the mechanical fibrillation stage.Lignin exhibits both promotion and inhibition effects on mechanical fibrillation, and the mutual competition between the two effects ultimately affects the energy consumption, morphology and yield of LCNFs. Furthermore, the recent research progress related to the contributions of lignin on the functional application of LCNFs was summarized, aiming to provide profound guidance for the preparation and application of LCNFs.

冷冻-萃取/真空干燥法制备坚固和耐疲劳的聚酰亚胺纤维气凝胶及其增强阻燃性复合材料

在现代新材料的快速发展中,用节能、省时、低成本和简便的新型方法制备具有优良机械性能和热学性能的轻质、低密度和高孔隙率气凝胶十分必要。在本工作中,我们使用短切电纺聚酰亚胺(PI)纤维作为支撑骨架,通过开发出一种无需特殊干燥方法的真空干燥(VD)与冷冻萃取相结合的方法,制备出高性能PI纤维气凝胶(PIFA)。所得PIFAs具有低密度(≤52.8 mg·cm^(-3))和高孔隙率(>96%)。该PIFA在至少20000次的循环压缩过程中展现出高度的耐疲劳性及低能量损失系数。密度为39.1 mg·cm^(-3)的PIFA具有40.4 mW·m^(-1)·K^(-1)的热导率。通过进一步使用聚硅氮烷对PIFA复合改性后,其具备更强的耐火性和氮气氛围中的高残留率(>70%)。这些优异的性能使PIFAs及其复合材料成为可应用于建筑工业、航空和航天工业轻质材料、隔热和防火层以及高温反应催化剂载体的可选材料。此外,本工作中提出的冷冻萃取/VD法因其节能、省时和节约成本而可拓展于制备其他材料。

Water Evaporation Triggered Self-Assembly of MXene on Non-Carbonized Wood with Well-Aligned Channels as Size-Customizable Free-Standing Electrode for Supercapacitors

Herein,non-carbonized wood-based electrodes and separators with well-aligned channels and excellent mechanical properties are developed for supercapacitors.To enhance the conductivity and boost the capacitance,Ti_(3)C_(2)(MXene)nanosheets with high electrical conductivity and excellent electrochemical activity are loaded into the wood cells via self-assembly triggered by fast evaporating water in Ti_(3)C_(2)suspension.By the assistance of positive charged polydopamine microspheres with large surface area,the self-restacking of Ti_(3)C_(2)nanosheets can be avoided and the high mass loading(50 wt%)can be achieved due to the extra driving force for Ti_(3)C_(2)absorption.Benefiting from the conductive Ti_(3)C_(2)nanosheets with massive active sites and the multiple well-aligned channels in wood with efficient transportation pathways for charge carriers,the as-designed free-standing electrode shows a large areal capacitance of 1060 mF cm^(-2)at 0.5 mA cm^(-2)and high capacitance retention of 67%at 10 mA cm^(-2).Also,this electrode is highly size-customizable,showing a good ability to be industrially processed into various shapes and dimensions.Furthermore,an all-wood based supercapacitor with Ti_(3)C_(2)/wood composites as two layers of electrodes and a wood slice as the separator is fabricated,presenting a high energy density of 10.5μW h cm^(-2)at 389.9μW cm^(-2).

Effects of Rice Straw Steam-explosion Spent Liquor on the Growth of Cabbage Seedlings

The direct use of spent liquor from pulping and papermaking engineering,which is abundant in active organic matter,can avoid resource wastage and environmental pollution.In this study,the effects of soaking solution and filtrate from steam-exploded rice straw on seed germination and the early development of cabbage were investigated.The results have shown that soaking solution and filtrate stimulated early cabbage growth at low concentrations.Optimal germination potential and the rate of soaking solution-treated cabbage seeds increased by 8%and 5%,respectively;meanwhile,that of the filtrate-treated cabbage seeds increased by 11%and 5%,respectively.Promotion of root growth by steam-exploded rice straw spent liquor was expressed in lateral root multiplication.The fresh weight of cabbage seedlings treated with the soaking solution/filtrate increased by more than 50%and the dry weight over 20%.Comparatively,the stimulation of filtrate on seed germination and early development of cabbage is superior to that of the soaking solution.Steam-exploded rice straw spent liquor is rich in bioactive lignin and oligosaccharides,which makes it a promising biostimulant for promoting crop growth.

^(1)H and ^(13)C NMR spectral assignments for low-concentration bile acids in biological samples

Bile acids are the main body of enterohepatic circulation in vivo.They have essential functions such as emulsifying fat,bacteriostasis and regulating multiple metabolic pathways as signal molecules.However,the assignments of NMR signals for some lowconcentration bile acids are still needed.This study combined 1D nuclear magnetic resonance(NMR)and 2D NMR techniques including 1He1H correlation spectroscopy(COSY),1He1H total correlation spectroscopy(TOCSY),1H J-resolved spectroscopy(J-Res),1He13C heteronuclear single quantum coherence spectroscopy(HSQC),and 1He13C heteronuclear multiple bond correlation spectroscopy(HMBC)to assign the 1H and 13C signals of six bile acids in aqueous solution at physiological pH(~7.4)and nine bile acids in methanol.These data are of importance to the NMR-based studies on lipid digestion,absorption,and metabolism.

Performance Analysis of RIS Assisted NOMA Networks over Rician Fading Channels

In this paper,we consider a downlink non-orthogonal multiple access(NOMA)network assisted by two reconfigurable intelligent surfaces(RISs)over Rician fading channels,in which each user communicates with the base station by the virtue of a RIS to enhance the reliability of the received signal.To evaluate the system performance of our proposed RIS-NOMA network,we first derive the exact and asymptotic expressions for the outage probability and ergodic rate of two users.Then,we derive the exact and asymptotic upper bound expressions for the ergodic rate of the nearby user.Based on asymptotic analytical results,the diversity orders for the outage probability and the high signal-to-noise ratio(SNR)slopes for the ergodic rate of the two users are obtained in the high SNR regime.Moreover,we derive the system throughputs of the proposed RIS-NOMA network in delay-limited and delay-tolerant transmission modes.Numerical results confirm our analysis and demonstrate that:1)The outage probability and ergodic rate of RIS-NOMA networks are superior to that of RIS-assisted orthogonalmultiple access(OMA)networks;2)The RIS-NOMA networks have ability to achieve a larger system throughput compared to RIS-OMA networks;and 3)The system performance of RIS-NOMA networks can be significantly improved as the number of reflecting elements and Rician factor increases.

纳米铂直接修饰玻碳电极的制备及在半胱氨酸中的电化学行为

采用一步化学原位还原法将球形纳米铂颗粒直接修饰在玻碳电极上,用SEM、EDS和电化学方法对该电极进行表征并与铂片电极、裸玻碳电极进行了对比。结果表明,纳米铂修饰电极的峰电流与扫描速度呈线性关系,纳米铂在电极表面覆盖率为1.28×10-7mol/cm2。循环伏安法研究结果表明纳米铂修饰电极对半胱氨酸的催化氧化作用和铂片电极相比提高了数倍,且峰电位负移了0.3V。在纳米铂修饰的玻碳电极上,半胱氨酸的浓度在1.0×10-7mol/L到1.0×10-5mol/L范围内和催化电流呈线性关系。

一种基于碳纳米管的色氨酸传感器

研究了色氨酸（tryptophan即Trp）在多壁碳纳米管修饰玻碳电极（MWNTs／GC）上的电化学行为。MWNTs／GC电极对Trp具有良好的电催化作用,相对于GC电极，Trp在MWNTs／GC上峰电位负移128mV，峰电流约为Gc电极上氧化峰电流的31倍。在1．0mol／LH2SO4中清洗能更新电极表面，消除产物吸附带来的影响。MWNTs／GC电极在含1．0×10^-4mol／L Trp的缓冲溶液中闭路富集2min时电流达到稳定值。研究了不同pH值影响的结果表明，参与电极反应的质子数和电子数相等。在pH=2．2时，Trp的氧化电流最大。利用LSV研究了电流与扫描速率的关系，结果表明，Trp在修饰电极上的氧化过程为扩散控制过程。在环境温度低于45℃时，随着温度增加，氧化电流逐渐增大。温度在16-35℃范围内,传感器的响应电流与温度成线性关系，温度系数为0．695μA／℃，说明此传感器在实测过程中因温度波动带来的测量误差很小。利用LSV研究了氧化峰电流与Trp的浓度关系的结果显示，峰电流与Trp的浓度在1．00×10^-6—1．00×10^-4moL／L范围内呈良好线性关系，检出限为1．82×10^-7mol／L（S／N=3）。该电极具有良好的灵敏度、选择性和稳定性,放置7d后，碳纳米管的峰电流仍能达到最初电流的98％。

Industry 5.0-The Relevance and Implications of Bionics and Synthetic Biology

Bionics （the imitation or abstraction of the ＂inventions＂ of nature） and, to an even greater extent, syn- thetic biology, will be as relevant to engineering development and industry as the silicon chip was over the last 50 years. Chemical industries already use so-called ＂white biotechnology＂ for new processes, new raw materials, and more sustainable use of resources. Synthetic biology is also used for the devel- opment of second-generation biofuels and for harvesting the sun＇s energy with the help of tailor-made microorganisms or biometrically designed catalysts. The market potential for bionics in medicine, en- gineering processes, and DNA storage is huge. ＂Moonshot＂ projects are already aggressively focusing on diseases and new materials, and a US-led competition is currently underway with the aim of creating a thousand new molecules. This article describes a timeline that starts with current projects and then moves on to code engineering projects and their implications, artificial DNA, signaling molecules, and biological circuitry. Beyond these projects, one of the next frontiers in bionics is the design of synthetic metabolisms that include artificial food chains and foods, and the bioengineering of raw materials; all of which will lead to new insights into biological principles. Bioengineering will be an innovation motor just as digitalization is today. This article discusses pertinent examples of bioengineering, particularly the use of alternative carbon-based biofuels and the techniques and perils of cell modification. Big data, analytics, and massive storage are important factors in this next frontier. Although synthetic biology will be as pervasive and transformative in the next 50 years as digitization and the Intemet are today, its ap- plications and impacts are still in nascent stages. This article provides a general taxonomy in which the development of bioengineering is classified in five stages （DNA analysis, bio-circuits, minimal genomes, protocells, xenobiology） from the familiar to the unknown, with implications for safety and security, in- dustrial development, and the development of bioengineering and biotechnology as an interdisciplinary field. Ethical issues and the importance of a public debate about the consequences of bionics and syn- thetic biology are discussed.