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Heterogeneous single-metal-site catalysts (HSMSCs) have been recognized as promising materials due to the advantages of evenly distributed active metal sites, easy separation, and recyclability. Herein, we construct a single-site Ru catalyst on porous ionic polymers (Ru/PIPs-IL3) via electrostatic interactions, which is a practical and useful strategy for synthesizing HSMSCs. The strong electrostatic interactions (Δ H = -73.4 and -83.5 kJ/mol for Ru-PPh 4 and Ru-P(vBn)(vPh) 3 , respectively) between the quaternary phosphonium cations and oxygen anions of the cyclopentadienyl ligand in Ru species were both consolidated by DFT calculation and X-ray crystallography. The XPS, ATR-IR, HAADF-STEM, and EXAFS analyses and ion exchange experiment were employed to characterize the structure of Ru/PIPs-IL3. These results provide compelling evidence that PIPs-IL3 can interact with Shvo's catalyst in a manner analogous to that observed with quaternary phosphonium (PPh 4 Cl), thereby anchoring the Ru through electrostatic interactions. Such heterogeneous single-site Ru catalyst Ru/PIPs-IL3 exhibited a twofold activity compared to the homogeneous catalyst with a TON CO of up to 545 and an excellent 98.5% CO selectivity in the low-temperature reverse water-gas shift reaction.

Backscattering losses (BSL), arising from intrinsic imperfections or unavoidable external perturbations in optical resonators, can severely impact photonic devices. In single-photon systems, robust quantum correlations against BSL remain largely unexplored despite their significance for various applications. Here, we demonstrate that single-photon blockade (SPB), a purely quantum effect, can be preserved against BSL by introducing a nanotip near a Kerr nonlinear resonator with intrinsic defects. Without the tip, BSL disrupts SPB, but tuning the tip's position restores robustness even under strong BSL. Notably, quantum correlations emerge while the classical mean photon number remains suppressed due to the interplay between resonator nonlinearity and tip-induced optical coupling. Our findings highlight nanoscale engineering as a powerful tool to protect and harness fragile quantum correlations, paving the way for robust single-photon sources and backscattering-immune quantum devices.

Palladium-catalyzed asymmetric hydrogenation of tetrasubstituted olefin 4-substituted 3-alkoxycar-bonylfuran-2(5 H )-ones was developed for the construction of 1,2-contiguous stereogenters, giving the chiral trans- 4-substituted 3-alkoxycarbonylbutyrolactone derivatives with up to 95% of enantioselectivities. The asymmetric hydrogenation reaction could proceed smoothly at gram scale without any loss of reactivity and enantioselectivity. In addition, the synthetic utility of the chiral reductive products has been demonstrated through useful building blocks.

The synthesis of high-purity gold nano bipyramids (Au NBPs) with a narrow size distribution and tunable plasmon resonances is of great significance for plasmon resonance-related applications. However, the synthesis Au NBP approach involves multiple steps with many parameters that can affect the purity of the final product. In this work, we were devoted to studying the effect of the molar ratio between hexadecyltrimethylammonium chloride (CTAC) and sodium citrate tribasic dihydrate (CiNa 3 ) on the seed formation stage. The results showed that the yield of Au NBP product has dramatically increased with the seed solution made from the molar ratio of CTAC:CiNa 3 at 21:1. Furthermore, using this optimal seed, we can efficiently synthesize Au NBPs with various sizes by adjusting the concentration of the seed but keeping the rest of the parameters constant. In this study, the longitudinal localized surface plasmon resonances (LSPRs) of Au NBPs exhibit tunability beyond 450 nm across the visible and near-infrared regions from 774 to 1224 nm. We were able to successfully fine-tune the LSPRs of Au NBPs in the spectral region to become resonant with the excitation wavelengths of an 808 nm near-infrared (NIR) laser. The photothermal activities of Au NBPs were studied under 808 nm laser irradiation at ambient conditions. The present work demonstrates a paradigm for the synthesis of Au NBPs with tunable LSPRs in a precise and controllable manner, achieved by examining the surfactant ratios in the formation of penta-twinned seeds., Competing Interests: The authors declare no competing financial interest., (© 2025 The Authors. Published by American Chemical Society.)

Affinity capture (AC) combined with mass spectrometry (MS)-based proteomics is highly utilized throughout the drug discovery pipeline to determine small-molecule target selectivity and engagement. However, the tedious sample preparation steps and time-consuming MS acquisition process have limited its use in a high-throughput format. Here, we report an automated workflow employing biotinylated probes and streptavidin magnetic beads for small-molecule target enrichment in the 96-well plate format, ending with direct sampling from EvoSep Solid Phase Extraction tips for liquid chromatography (LC)-tandem mass spectrometry (MS/MS) analysis. The streamlined process significantly reduced both the overall and hands-on time needed for sample preparation. Additionally, we developed a data-independent acquisition-mass spectrometry (DIA-MS) method to establish an efficient label-free quantitative chemical proteomic kinome profiling workflow. DIA-MS yielded a coverage of ∼380 kinases, a > 60% increase compared to using a data-dependent acquisition (DDA)-MS method, and provided reproducible target profiling of the kinase inhibitor dasatinib. We further showcased the applicability of this AC-MS workflow for assessing the selectivity of two clinical-stage CDK9 inhibitors against ∼250 probe-enriched kinases. Our study here provides a roadmap for efficient target engagement and selectivity profiling in native cell or tissue lysates using AC-MS.

Sodium antiperovskite materials (APs) are a promising class of solid-state electrolytes owing to their high structural tolerance and good formability. However, few APs have been synthesized experimentally, indicating the necessity of exploring potential chemical spaces with higher ionic conductivities. Herein, through a combined particle swarm optimization algorithm, high-throughput first-principles calculations, ab initio molecular dynamics, and long time-scale machine-learning molecular dynamics simulations, strategies based on site-exchanging and anion clusters are shown to simultaneously enhance the thermal stability and sodium diffusivity in the designed APs. Among these APs, the highest theoretical ionic conductivity of 39.05 mS/cm is achieved with Na 3 BrSO 4 at room temperature due to the strong coupling of cluster rotation and sodium migration. We highlight that not only the rotation dynamics but also its coupling with Na diffusion contribute to the high ionic conductivity, as confirmed by the proposed local difference frequency center to evaluate the coupling degree. Our work designs promising site-exchanging APs and offers insights into the coupling between anion rotation and cation migration, which can effectively guide the design of superionic conductors with cluster rotation dynamics.

As environmental energy harvesting gains increasing importance in self-powered systems and large-scale energy demands, wind energy, as a clean, pollution-free, and renewable source, has garnered widespread attention. However, achieving efficient wind energy collection remains challenging. This study proposes a high-performance rotating structure triboelectric-electromagnetic hybrid nanogenerator designed for environmental wind energy harvesting. By optimizing the magnetic circuit design of the electromagnetic generator, the dispersed radial magnetic field is converted into a unified axial magnetic field, enabling efficient power generation with only a single annular coil, thereby simplifying the generator design and reducing manufacturing and maintenance costs. Additionally, a triboelectric nanogenerator design with soft contact friction between polycarbonate (PC) fur and fluorinated ethylene propylene (FEP) film was implemented, optimizing the spacing between the electrode and friction layers, thus enhancing output performance and device durability. Furthermore, we simulated and experimentally tested the output waveform of the designed hybrid generator structure, with the results showing a high degree of similarity, further validating the rationality of the device design and providing guidance for structural optimization. Subsequently, we achieved efficient energy storage using an energy management circuit (EMC). With the integration of the EMC, the generator successfully powered a Bluetooth temperature and humidity sensor at a wind speed of 10 m/s, achieving wireless transmission, and demonstrating its potential application in traffic signal systems and other natural environmental systems. This research provides an important reference for further exploration of novel wind energy harvesting technologies.

The notorious collapse of the electrode structure and strong electrostatic interactions in aqueous zinc-ion batteries (AZIBs) limit the achievement of a long cycle life. Herein, by designing an ordered/disordered hybrid structure, we have effectively preserved the integrity of the V 2 O 5 ·1.6H 2 O (VOH) electrode. Moreover, our approach facilitates the release of stress concentration contributed to by the amorphous component, alleviating the strong electrostatic interaction merited by crystal water and promoting the diffusion kinetics of Zn 2+ assisted by the crystalline component. Noteworthy, the crystal water serves as an interlayer pillar significantly enhancing the structural stability of the electrode. As a result, our VOH electrode exhibits high electrochemical performance. It delivered 227.8 mAh g -1 at a higher current density of 2 A g -1 , and a high cycle life of 1000 cycles with 95% capacity retention was achieved at a current density of 1 A g -1 .

In recent years, the rapid advancement of flexible conductive materials has significantly increased the demand for dough materials that offer high flexibility and conductivity for diverse applications. Here, we developed a flexible, stretchable, and self-healing dough utilizing hydrogen-bonding interactions between glutathione-stabilized copper nanoclusters (GSH-Cu NCs) and poly(acrylic acid) (PAA). The dough materials can be kneaded, readily reshaped, and further processed to create bulk materials of arbitrary form factors. The incorporation of PAA not only preserved the vibrant blue emission of GSH-Cu NCs but also enhanced their electrical conductivity and stretchability. The dough can be stretched up to 25 times its initial length and achieves complete self-healing in a short time. Moreover, the dough can automatically repair physical damage and return to its initial conductivity levels after healing. Surprisingly, the electrical conductivity of the dough can reach as high as 2.97 S/m, which is relatively superior compared to that of conventional conductive materials. This study presents a dough that serves as a highly sensitive strain sensor, capable of effectively monitoring human movement across a broad range of strains.

We utilize molecular dynamics simulations to comparably investigate the wetting and motion behavior of droplets on liquid-like surfaces (LLS) with varying grafting conditions. Polydimethylsiloxane (PDMS) and perfluoropolyether (PFPE) have been considered to be flexible molecules versus rigid molecules of trichloro(octadecyl) silane (OTS) and trichloro(1H,1H,2H,2H-perfluorooctyl) silane (PFOS), respectively. Our findings reveal that droplets on surfaces tethered with either PDMS or PFPE brushes can generate indentations and wetting ridges, providing microscopic evidence of their liquid-like nature. The grafting density of mobile chains exerts a dominant influence on the wetting properties compared to the molecular weight. A parameter map is created to pinpoint the precise range of grafting densities essential for the optimal construction of LLS at predetermined molecular weights. Furthermore, the investigation of droplet motion dynamics on LLS demonstrates that droplets consistently exhibit a rolling state, regardless of the intensity of the applied lateral force. The movement pattern of the droplet shifts only under conditions where the grafting density is significantly reduced and the substrate exhibits hydrophilic tendencies. These findings and the developed model are anticipated to offer valuable guidelines for optimal designs of LLS.

β-Amino nitriles are important molecular scaffolds. Cyanoalkylation of imines is the most straightforward method for the construction of these scaffolds. In this study, we report the novel cyanoalkylation of imines via radical coupling enabled by a photoactive electron donor-acceptor complex. This strategy is characterized by mild conditions, broad reaction scopes, and high atom economy. The scalability and practicality of this strategy are demonstrated by a 40 g continuous flow system from which a variety of important pharmaceutical-related molecules were obtained.

Spirocyclic compounds are abundant in biologically active products. However, the divergent synthesis of spirocyclic compounds using low-cost and abundant available starting materials remains a challenge. Herein, we report an effective method for producing spirocyclic motifs using a cyclic β-carbonyl ester or amide and ethylene via thianthrenation. This strategy highlights the exciting possibility of utilizing abundant ethylene as a C-2 synthon and allows regulating the core structure of the spirocyclic compound by simply altering the base type.

In this work, we report a facile emulsion swelling route to prepare surface-wrinkled silica-polystyrene (SiO 2 -PS) composite particles. Submicrometer-sized, near-spherical SiO 2 -PS composite particles were first synthesized by dispersion polymerization of styrene in an ethanol/water mixture, and then, surface-wrinkled SiO 2 -PS particles were obtained by swelling the SiO 2 -PS particles with a toluene/water emulsion and subsequent drying. It is emphasized that no surface pretreatment on the SiO 2 -PS composite particles is required for the formation of the wrinkled surface, and the most striking feature is that the surface-wrinkled particle was not deformed from a single near-spherical SiO 2 -PS composite particle but from many ones. The influence of various swelling parameters including toluene/particle mass ratio, surfactant concentration, stirring rate, swelling temperature, swelling time, and silica size on the morphology of the composite particles was studied. This method represents a new paradigm for the preparation of concave polymer colloids.

A scene that contains both old and instant events with a clear motion trail is visually intriguing and dynamic, which can convey a sense of change, transition, or evolution. Developing an eco-friendly delay display system offers a powerful tool for fusing old and instant events, which can be used for visualizing motion trails. Herein, we brighten triplet excitons of carbon nanodots (CNDs) and increase their emission yield by a multidimensional confinement strategy, and the CND-based delay display array is demonstrated. The intense confinement effects via multidimensional confinement strategy suppress nonradiative transitions, and 240% enhancement in the phosphorescence efficiency and 260% enhancement in the lifetime of the CNDs are thus realized. Considering their distinctive phosphorescence performances, a delay display array containing a 4 × 4 CND-based delay lighting device is demonstrated, which can provide ultralong phosphorescence over 7 s, and the motion that occurred in different timelines is recorded clearly. This finding will motivate the investigation of phosphorescent CNDs in motion trail recognition.

Multitarget medications represent an appealing therapy against the disease with multifactorial abnormalities─cancer. Therefore, simultaneously targeting son of sevenless 1 (SOS1) and epidermal growth factor receptor (EGFR), two aberrantly expressed proteins crucial for the oncogenesis and progression of prostate cancer, may achieve active antitumor effects. Here, we discovered dual SOS1/EGFR-targeting compounds via pharmacophore-based docking screening. The most prominent compound SE-9 exhibited nanomolar inhibition activity against both SOS1 and EGFR and efficiently suppressed the phosphorylation of ERK and AKT in prostate cancer cells PC-3. Cellular assays also revealed that SE-9 displayed strong antiproliferative activities through diverse mechanisms, such as induction of cell apoptosis and G1 phase cell cycle arrest, as well as reduction of angiogenesis and migration. Further in vivo findings showed that SE-9 potently inhibited tumor growth in PC-3 xenografts without obvious toxicity. Overall, SE-9 is a novel dual-targeting SOS1/EGFR inhibitor that represents a promising treatment strategy for prostate cancer.

Phosphogypsum produced from wet-processed phosphoric acid mainly consists of calcium sulfate dihydrate, which is an important sulfur resource. The traditional sulfuric acid and cement process based on phosphogypsum suffers from unstable cement quality owing to impurities such as phosphorus and fluorine and kiln ringing caused by the low-melting phase. This study investigated sulfur recovery and value-added utilization of liquid slag from high-silica phosphogypsum via carbothermal reduction smelting. A phosphogypsum ingredient (PGI) system was constructed by adding appropriate amounts of silica, alumina, magnesium oxides, and iron oxides to meet the production requirements of slag wool. Carbothermal reduction smelting experiments suggested that the temperature and C/S molar ratio significantly affected the desulfurization rate and phase structure of the slag. More than 97.44 wt % of sulfur could be recovered with a C/S molar ratio of 0.5-0.8 at 1300 °C or above in the molten state, and the molten slag was an amorphous magnesium-calcium-aluminosilicate. The PGI desulfurization mechanism is discussed based on the phase transformation and slag microstructure evolution., Competing Interests: The authors declare no competing financial interest., (© 2024 The Authors. Published by American Chemical Society.)

Amorphous materials disrupt the intrinsic linear scalar dependence seen in their crystalline counterparts, typically exhibiting enhanced catalytic characteristics. Nevertheless, substantial obstacles remain in terms of boosting their stability, enhancing their conductivity, and elucidating distinct catalytic mechanisms. Herein, a core-shell catalyst, comprising a crystalline SnO 2 core and an amorphous SnO x shell supported on MXene (denoted as SnO 2 @SnO x /MXene), was prepared utilizing hydrothermal and solution reduction methods. The SnO 2 @SnO x /MXene catalyst excels in the electrocatalytic conversion of CO 2 to formate, yielding a Faradaic efficiency (FE) as high as 93% for formate production at -1.17 V vs RHE and demonstrating exceptional durability. Both density functional theory (DFT) calculations and experimental results indicate that the SnO x shell bolsters formate formation by fine-tuning the adsorption energy of the *OCHO intermediate. In SnO 2 @SnO x /MXene, MXene plays a vital role in enhancing the conductivity and stability of the amorphous shell and especially amplifying Raman signals of catalyst components. The ex/in situ surface-enhanced Raman scattering (SERS) application further confirms the formation of amorphous SnO x and further enables the direct detection of the formation of the intermediate species. This work provides the basis for the application of amorphous materials in practical electrocatalytic reduction of CO 2 reduction.

Herein, we describe a metal-free approach for the cross-coupling of arenes or styryl-thianthrenium salts (TTs) with diarylphosphines via an electron donor-acceptor (EDA) complex. Various tertiary phosphines were obtained with high site selectivity and good functional group tolerance. This method enables straightforward construction of C-P bonds via C-H activation of arenes and allows the late-stage functionalization of natural products or pharmaceutical molecules. Mechanistic studies support the approach involving a photoinduced EDA complex.

The complexity of the evolution of the permeability of coal is determined by the reservoir structure. Further, there exists an interaction between the fracture matrix, which further complicates changes in permeability. When the actual mining conditions of a coal mine are considered, a permeability model that considered the combined effects of stress, gas adsorption, and temperature was proposed. Subsequently, the model is verified by published test data. Based on the analysis of permeability, a calculation model of the slip coefficient that considered the combined effects of stress, gas adsorption, and temperature is proposed. With respect to this, any change in the slippage coefficient is only determined by the width of the fracture channel, which affected the flow of coal gas. In the process of a temperature increase, the slip coefficient tends to increase and the larger effective stress corresponds to a larger slip coefficient. In addition, under constant-temperature conditions, we also discuss the evolution of coal permeability and the variation of the coal gas slippage factor under different boundary conditions through the proposed model. This study aims to further the understanding of the seepage characteristics and slippage effects of coalbed methane, which would have a positive impact on the mining of coal., Competing Interests: The authors declare no competing financial interest., (© 2023 The Authors. Published by American Chemical Society.)

Left-sided and right-sided colon cancer (LSCC and RSCC) display different biological and clinical characteristics. However, the differences in their tumorigenesis and tumor microenvironment remain unclear. In this study, we profiled the proteomic landscapes of LSCC and RSCC with data-independent acquisition mass spectrometry (DIA-MS) using fresh tumor and adjacent normal tissues from 24 patients. A total of 7403 proteingroups were primarily identified with DIA-MS. After quality control, 7212 proteingroups were used for further analysis. Through comparing the difference in proteomic profiles between LSCC and RSCC samples, 2556 commonly and 1982 region-type-specific regulated proteingroups were characterized. During the development of LSCC and RSCC, metabolic, growth, cell division, cell adhesion, and migration pathways were found to be significantly dysregulated ( P < 0.05), which was further confirmed by transcriptome data from TCGA. Compared to RSCC, most parts of the immune-related signatures, immune cell infiltration scores, and overall immune scores of LSCC were higher. The systematic elucidation of proteomic and transcriptomic profiles in this work improves our understanding of tumorigenesis and immune microenvironment characteristics of LSCC and RSCC.

Bimolecular or tetramolecular G-quadruplexes (GQs) are predominantly self-assembled by the same sequence-identical G-rich oligonucleotides and usually remain inert to the strand displacement reaction (SDR) with other short G-rich invading fragments of DNA or RNA. Appealingly, in this study, we demonstrate that a parallel homomeric bimolecular GQ target of Tub10 d(CAGGGAGGGT) as the starting reactant, although completely folded in K + solution and sufficiently stable (melting temperature of 57.7 °C), can still spontaneously accept strand invasion by a pair of short G-rich invading probes of P1 d(TGGGA) near room temperature. The final SDR product is a novel parallel heteromeric trimolecular GQ (tri-GQ) of Tub10 / 2P1 reassembled between one Tub10 strand and two P1 strands. Here we present, to the best of our knowledge, the first NMR solution structure of such a discrete heteromeric tri-GQ and unveil a unique mode of two probes vs one target in mutual recognition among G-rich canonical DNA oligomers. As a model system, the short invading probe P1 can spontaneously trap G-rich target Tub10 from a Watson-Crick duplex completely hybridized between Tub10 and its fully complementary strand d(ACCCTCCCTG). The Tub10 sequence of d(CAGGGAGGGT) is a fragment from the G-rich promoter region of the human β2-tubulin gene. Our findings provide new insights into the Hoogsteen pairing-based SDR between a GQ target and double invading probes of short G-rich DNA fragments and are expected to grant access to increasingly complex architectures in GQ-based DNA nanotechnology.

A unique transition-metal-free radical thiolation of 2-azaallyl anions has been developed. Easily accessible thiosulfonates and 2-azaallyls undergo the tandem process of single-electron transfer and radical-radical coupling to construct C(sp 3 )-S bonds. This robust protocol enables a mild and chemoselective coupling between 2-azaallyl anions and thiosulfonates to access α-amino sulfides in 50-92% yields (25 examples). The scalability of this protocol was demonstrated by telescopic gram-scale experiments. Mechanistic studies provide significant evidence for this radical thiolation reaction.

Quantum dot (QD)-organic dye couple chromophores are topical due to their applications in biology, catalysis, and energy. The maximization of energy transfer efficiency can be guided by the underlying Förster or Dexter mechanisms; however, the impact of fluorescence intermittency must also be considered. Here we demonstrate that the average ⟨ t on ⟩ and ⟨ t off ⟩ times of dye acceptors in coupled QD-dye chromophores are substantially affected by the donors' blinking behavior. With regard to biological imaging, this effect beneficially minimizes the photobleaching of the acceptor dye. The implications for alternative energy are less encouraging as the acceptors' capacity to store energy, using ⟨ t on ⟩/⟨ t off ⟩ as a metric, was reduced by as much as ∼95%. These detrimental effects can be mitigated by suppressing QD blinking via surface treatment. This study also demonstrates several instances of the nonconformity of QD blinking dynamics to a power law distribution, as a robust examination of the off times reveals log-normal behavior that is consistent with the Albery model.

The multi-redox mechanism involving multi-sites has great implications to dictate the catalytic water oxidation. Understanding the sequential dynamics of multi-steps in oxygen evolution reaction (OER) cycles on working catalysts is a highly important but challenging issue. Here, using quasi-operando transient absorption (TA) spectroscopy and a typical photosensitization strategy, we succeeded in resolving the sequential oxidation kinetics involving multi-active sites for water oxidation in OER catalytic cycle, with Co 3 O 4 nanoparticles as model catalysts. When OER initiates from fast oxidation of surface Co 2+ ions, both surface Co 2+ and Co 3+ ions are active sites of the multi-cobalt centers for water oxidation. In the sequential kinetics (Co 2+ → Co 3+ → Co 4+ ), the key characteristic is fast oxidation and slow consumption for all the cobalt species. Due to this characteristic, the Co 4+ intermediate distribution plays a determining role in OER activity and results in the slow overall OER kinetics. These insights shed light on the kinetic understanding of water oxidation on heterogeneous catalysts with multi-sites.

Touch panels based on ionic conductive hydrogels perform excellent flexibility and biocompatibility, becoming promising candidates for the next-generation human-machine interface. However, these ionic hydrogels are usually composed of cross-linked polymeric networks that are difficult to be recycled or reconfigured, resulting in environmental issues. Herein, we designed a lithium ion-triggered gelation strategy to provide a conductive molecular hydrogel with thixotropy, which can be mechanically recycled or reconfigured at room temperature. In this hydrogel, lithium ions function as ionic bridges to construct supramolecular nanoassemblies and charge carriers to impart ionic conductivity. With polymer additives, the mechanical accommodability of the hydrogel was improved to meet the requirements of the daily use of touch panels. When this molecular hydrogel was fabricated into a surface capacitive touch panel, real-time sensing and reliable touch locating abilities were achieved. Remarkably, this touch panel can be reconfigured into 1D, 2D, and 3D device structures by a simple stirring-remolding method under ambient conditions. This work brings new insight into enriching the functionalities of hydrogel-based ionotronics with a supramolecular approach.

A panchromatic triad and a charge-separation unit are joined in a crossbar architecture to capture solar energy. The panchromatic-absorber triad (T) is comprised of a central free-base porphyrin that is strongly coupled via direct ethyne linkages to two perylene-monoimide (PMI) groups. The charge-separation unit incorporates a free-base or zinc chlorin (C or ZnC) as a hole acceptor (or electron donor) and a perylene-diimide (PDI) as an electron acceptor, both attached to the porphyrin via diphenylethyne linkers. The free-base porphyrin is common to both light-harvesting and charge-separation motifs. The chlorin and PDI also function as ancillary light absorbers, complementing direct excitation of the panchromatic triad to produce the discrete lowest excited state of the array (T*). Attainment of full charge separation across the pentad entails two steps: (1) an initial excited-state hole/electron-transfer process to oxidize the chlorin (and reduce the panchromatic triad) or reduce the PDI (and oxidize the panchromatic triad); and (2) subsequent ground-state electron/hole migration to produce oxidized chlorin and reduced PDI. Full charge separation for pentad ZnC-T-PDI to generate ZnC + -T-PDI - occurs with a quantum yield of ∼30% and mean lifetime ∼1 μs in dimethyl sulfoxide. For C-T-PDI , initial charge separation is followed by rapid charge recombination. The molecular designs and studies reported here reveal the challenges of balancing the demands for charge separation (linker length and composition, excited-state energies, redox potentials, and medium polarity) with the constraints for panchromatic absorption (strong electronic coupling of the porphyrin and two PMI units) for integrated function in solar-energy conversion.

Microbial-based iron reduction is an emerging technology used as an alternative to conventional chemical-based iron reduction. The iron reduction in kaolin refinement is vital for enhancing its commercial value. Extensive studies on microbial-based iron reduction mainly focus on Gram-negative bacteria, whereas little is understood about Gram-positive bacteria's mechanism and potential application. This study aims to investigate the iron-reducing mechanism of two Gram-positive bacterial isolates, Bacillus cereus ( B. cereus ) and Staphylococcus aureus ( S. aureus ). By varying the growth environment of bacteria and monitoring the biochemical changes during the process of iron reduction, the results show that Gram-positive bacterial iron reduction performance depends on the medium composition, differing from Gram-negative bacteria-based reduction processes. Nitrogen-rich medium facilitates the microbial basification of the medium, where the alkaline conditions impact the microbial iron reduction process by altering the gene expression involved in intracellular pH homeostasis and microbial growth. This discovery will contribute to the mineral refining processes and promote the development of microbial-based bioprocesses for ore purification, while also laying the foundation for investigating other Gram-positive bacterial iron-reducing ability., Competing Interests: The authors declare no competing financial interest., (© 2022 The Authors. Published by American Chemical Society.)

A critical bottleneck for realizing an efficient Schottky type Si photoelectrode is minimizing the charge extraction losses across the heterointerface via reducing the unfavorite defects. This requires a clear microscopic insight into the correlation between interfacial features and photoconversion. Herein, by taking the n-Si/oxide (MO x )/Ni as the prototype, the heterointerface with the different characteristics and its effects on charge transportation and the corresponding photoelectric/photoelectrochemical (PEC) behaviors were clarified. An ultra-thin AlO x layer can effectively diminish the interfacial pinning of n-Si/Ni and significantly facilitate the photoconversion; meanwhile, it results in some unexpected donor-like deep defects at around 0.59 eV below the conduction band of n-Si, which could be ionized under a reverse bias and cause about 10% photogenerated charge recombination. Fortunately, these deep defects can be further eliminated by cooperating AlO x with a thin Au layer. The AlO x /Au dual-interlayer can remove almost all unexpected defects and maximize the efficiency of the electric field for charge extraction from semiconductor Si for the surface catalytic reaction. Eventually, the n-Si/SiO x /AlO x /Au/Ni/NiFeO x photoanode exhibited a record fill factor of 0.75 for the corresponding photoelectric device and an applied bias photon-to-current efficiency of 3.71% for PEC water oxidation. This study provides definite insights into interfacial electronic states and elaborates their crucial role in solar photoelectric conversion.

The impact of vibrational-electronic resonances on the rate of excited-state energy transfer is examined in a set of bacteriochlorin dyads that employ the same phenylethyne linker. The donor/acceptor excited-state energy gap is tuned from ∼200 to ∼1100 cm -1 using peripheral substituents on the donor and acceptor bacteriochlorin macrocycles. Ultrafast energy transfer is observed with rate constants of (0.3 ps) -1 to (1.7 ps) -1 , which agree with those predicted by Förster theory to within a factor of 2. Furthermore, the measured rates follow a trend-line with only small deviations that do not correlate with the density of vibrations at the donor/acceptor excited-state energy gap. Thus, if vibrational-electronic resonances occur in any of these dyads, which seems likely, the impact on the rate of energy transfer is small.

Dendritic cells (DCs) can infiltrate tight junctions of the epithelium to collect remote antigens during immune surveillance. While elongated membrane structures represent a plausible structure to perform this task, their functional mechanisms remain elusive owing to the lack of high-resolution characterizations in live DCs. Here, we developed fluorescent artificial antigens (FAAs) based on quantum dots coated with polyacrylic acid. Single-particle tracking of FAAs enables us to superresolve the membrane fiber network responsible for the antigen uptake. Using the DC2.4 cell line as a model system, we discovered the extensive membrane network approaching 200 μm in length with tunnel-like cavities about 150 nm in width. The membrane fiber network also contained heterogeneous circular migrasomes. Disconnecting the membrane network from the cell body decreased the intracellular FAA density. Our study enables mechanistic investigations of DC membrane networks and nanocarriers that target this mechanism.

Herein is introduced the application of "super-electron-donor"(SED) 2-azaallyl anions in a tandem reduction/radical cyclization/radical coupling/aromatization protocol that enables the rapid construction of isoquinolines. The value of this transition-metal-free method is highlighted by the wide range of isoquinoline ethyl amines prepared with good functional group tolerance and yields. An operationally simple gram scale synthesis is also conducted, confirming the scalability.

Ligands are the most commonly used means to control the regioselectivity of organic reactions. It is very important to develop new regioselective control methods for organic synthesis. In this study, we designed and synthesized a single-atomic-site catalyst (SAC), namely, Cu1-TiC, with strong electronic metal-support interaction (EMSI) effects by studying various reaction mechanisms. π cloud back-donation to the alkyne on the metal catalytic intermediate was enhanced during the reaction by using transient electron-rich characteristics. In this way, the reaction achieved highly linear- E -type regioselective conversion of electronically unbiased alkynes and completely avoided the formation of branched isomers (ln:br >100:1, TON up to 612, 3 times higher than previously recorded). The structural elements of the SACs were designed following the requirements of the synthesis mechanism. Every element in the catalyst played an important role in the synthesis mechanism. This demonstrated that the EMSI, which is normally thought to be responsible for the improvement in catalytic efficiency and durability in heterogeneous catalysis, now first shows exciting potential for regulating the regioselectivity in homogeneous catalysis.

Recently, electrochemical NO reduction (eNORR) to ammonia has attracted enormous research interests due to the dual benefits in ammonia synthesis and denitrification fields. Herein, taking Ag as a model catalyst, we have developed a microkinetic model to rationalize the general selectivity trend of eNORR with varying potential, which has been observed widely in experiments, but not understood well. The model reproduces experiments well, quantitatively describing the selectivity turnover from N 2 O to NH 3 and from NH 3 to H 2 with more negative potential. The first turnover of selectivity is due to the thermochemical coupling of two NO* limiting the N 2 O production. The second turnover is attributed to the larger transfer coefficient (β) of HER than NH 3 production. This work reveals how electrode potential regulate the selectivity of eNORR, which is also beneficial to understand the commonly increasing HER selectivity with the decrease of potential in some other electroreduction reactions such as CO 2 reduction.

Surface-modified mesoporous silica nanoparticles (MSNs) have attracted more and more attention as promising materials for biomolecule delivery. However, the lack of detailed evaluation relevant to the potential cytotoxicity of these MSNs is still a major obstacle for their applications. Unlike the bare MSNs and amino- or liposome-modified MSNs, we found that polyethylenimine-modified MSNs (MSNs-PEI) had no obvious toxicity to human umbilical vein endothelial cells (HUVECs) at the concentrations up to 100 μg/mL. However, MSNs-PEI induced autophagosomes accumulation by blocking their fusion with lysosomes, an essential mechanism for the cytotoxicity of many nanoparticles (NPs). Thus, we predicted that an alternative pathway for autophagosome clearance exists in HUVECs to relieve autophagic stress induced by MSNs-PEI. We found that MSNs-PEI prevented STX17 loading onto autophagosomes instead of influencing lysosomal pH or proteolytic activity. MSNs-PEI induced the structural alternation of the cytoskeleton but did not cause endoplasmic reticulum stress. The accumulated autophagosomes were released to the extracellular space via microvesicles (MVs) when the autophagic degradation was blocked by MSNs-PEI. More importantly, blockade of either autophagosome formation or release caused the accumulation of damaged mitochondria and excessive ROS production in the MSNs-PEI-treated HUVECs, which in turn led to cell death. Thus, we propose here that the MV-mediated autophagosome release, a compensation mechanism, allows the vascular endothelial cell survival when the degradation of autophagosomes is blocked by MSNs-PEI. Accordingly, promoting the release of accumulated autophagosomes may be a protective strategy against the endothelial toxicity of NPs.

Here we report a unique transition-metal-free C(sp 3 )-H/C(sp 3 )-H coupling of cycloalkanes at room temperature. Unactivated cycloalkanes and 2-azaallyls underwent the combination process of single-electron transfer (SET) and hydrogen atom transfer (HAT) to deliver a wide variety of cycloalkane-functionalized products. This expedient approach enables C(sp 3 )-H/C(sp 3 )-H coupling of cycloalkanes under mild conditions without transition metals, initiators, and oxidants.

The physical and chemical properties of MXenes are strongly dependent on surface terminations; thus, the tailoring of surface functional groups in two-dimensional transition-metal carbides (MXenes) may extend the applicability of these compelling materials to a wider set of fields. In this work, we demonstrate the chemical modification of Ti 3 C 2 T x MXene via diazonium covalent chemistry and the subsequent effects on the electrical properties of MXene. The 4-nitrophenyl group was grafted onto the surface of MXene through a solid-liquid reaction, which was confirmed by various characterization methods, including X-ray photoelectron spectroscopy, Fourier transform infrared spectroscopy, electron energy loss spectroscopy, atomic force microscopy, and transmission electron microscopy. The degree of modification of MXene is expediently tunable by adjusting the concentration of the diazonium salt solution. The work function of functionalized MXene is modifiable by regulating the quantity of grafted diazonium surface groups, with an adjustable range of around 0.6 eV. Further, in this study, the electrical properties of modified MXene are investigated through the fabrication of field-effect-transistor devices that utilize modified MXene as a channel material. It was demonstrated that with increasing concentration of 4-nitrophenyl groups grafted onto the surface the on/off current ratio of the modified MXene was improved to as much as 3.56, with a corresponding decrease in conductivity and mobility. The proposed approach of controlled modification of surface groups in Ti 3 C 2 T x may imbue Ti 3 C 2 T x with favorable electronic behaviors and demonstrate prospects for use in electronic field applications.

The membraneless organelles (MLOs) and coacervates of oppositely charged polyelectrolytes are both formed by liquid-liquid phase separation. To reveal how the crowded cell interior regulates the MLOs, we chose the coacervates formed by peptide S5 and single-stranded oligonucleotide (ss-oligo) at 1:1 charge ratio and investigated the phase separation processes in polyacrylamide (PAM) and poly(ethylene oxide) (PEO) media at varying concentrations. Results show that the droplet formation unit is the neutral primary complex, instead of individual S5 or ss-oligo. Therefore, the coacervation process can be described by the classic theory of nucleation and growth. The dynamic scaling relationships show that S5/ss-oligo coacervation undergoes in sequence the heterogeneous nucleation, diffusion-limited growth, and Brownian motion coalescence with time. The inert crowders generate multiple effects, including accelerating the growth of droplets, weakening the electrostatic attraction, and slowing down or even trapping the droplets in the crowder network. The overall effect is that both the size and size distribution of the droplets decrease with increasing crowder concentration, and the effect of PEO is stronger than that of PAM. Our study provides a further step toward a deeper understanding of the kinetics of MLOs in crowded living cells.

Flexible optoelectronic devices attract considerable attention due to their prominent role in creating novel wearable apparatus for bionics, robotics, health care, and so forth. Although bulk single-crystalline perovskite-based materials are well-recognized for the high photoelectric conversion efficiency than the polycrystalline ones, their stiff and brittle nature unfortunately prohibits their application for flexible devices. Here, we introduce ultrathin single-crystalline perovskite film as the active layer and demonstrate a high-performance flexible photodetector with prevailing bending reliability. With a much-reduced thickness of 20 nm, the photodetector made of this ultrathin film can achieve a significantly increased responsivity as 5600A/W, 2 orders of magnitude higher than that of recently reported flexible perovskite photodetectors. The demonstrated 0.2 MHz 3 dB bandwidth further paves the way for high-speed photodetection. Notably, all its optoelectronic characteristics resume after being bent over thousands of times. These results manifest the great potential of single-crystalline perovskite ultrathin films for developing wearable and flexible optoelectronic devices.

Non-Hermitian systems, with symmetric or antisymmetric Hamiltonians under the parity-time (PT) operations, can have entirely real or imaginary eigenvalues. This fact has led to surprising discoveries such as loss-induced lasing and topological energy transfer. A merit of anti-PT systems is free of gain, but in recent efforts on making anti-PT devices, nonlinearity is still required. Here, counterintuitively, we show how to achieve anti-PT symmetry and its spontaneous breaking in a linear device by spinning a lossy resonator. Compared with a Hermitian spinning device, significantly enhanced optical isolation and ultrasensitive nanoparticle sensing are achievable in the anti-PT-broken phase. In a broader view, our work provides a new tool to study anti-PT physics, with such a wide range of applications as anti-PT lasers, anti-PT gyroscopes, and anti-PT topological photonics or optomechanics.

As a member of the sirtuin family of enzymes, SIRT2 promotes tumor growth and regulates various biological pathways through lysine deacetylation and defatty-acylation. In the past few years, many SIRT2-selective small molecule inhibitors have been developed, but none have demonstrated simultaneous inhibition of both SIRT2 activities in cells. To further scrutinize the physiological importance and significance of SIRT2 deacetylase and defatty-acylase activities, small molecules that can selectively inhibit both activities of SIRT2 in living cells are needed. Here, we have applied the Proteolysis Targeting Chimera (PROTAC) strategy and synthesized a new SIRT2 inhibitor (TM-P4-Thal) to degrade SIRT2 selectively, which led to simultaneous inhibition of its deacetylase and defatty-acylase activities in living cells. Additionally, this compound exemplifies the advantage of the PROTAC strategy that allows complete eradication of an enzyme and its activity in biological settings., Competing Interests: The authors declare no competing financial interest.

Construction of protocells with hierarchical structures and living functions is still a great challenge. Growing evidence demonstrates that the membraneless organelles, which facilitate many essential cellular processes, are formed by RNA, protein, and other biopolymers via liquid-liquid phase separation (LLPS). The formation of the protocell in the early days of Earth could follow the same principle. In this work, we develop a novel coacervate-based protocell containing membraneless subcompartments via spontaneous liquid-liquid phase separation by simply mixing single-stranded oligonucleotides (ss-oligo), quaternized dextran (Q-dextran), and poly(l-lysine) (PLL) together. The resulting biphasic droplet, with PLL/ss-oligo phase being the internal subcompartments and Q-dextran/ss-oligo phase as the surrounding medium, is capable of sequestering and partitioning biomolecules into distinct regions. When the droplet is exposed to salt or Dextranase, the surrounding Q-dextran/ss-oligo phase will be gradually dissociated, resulting in the chaotic movement and fusion of internal subcompartments. Besides, the external electric field at a lower strength can drive the biphasic droplet to undergo a deviated circulation concomitant with the fusion of localized subcompartments, while a high-strength electric field can polarize the whole droplet, resulting in the release of daughter droplets in a controllable manner. Our study highlights that liquid-liquid phase separation of biopolymers is a powerful strategy to construct hierarchically structured protocells resembling the morphology and functions of living cells and provides a step toward a better understanding of the transition mechanism from nonliving to living matter under prebiotic conditions.

We have carried out coarse-grained molecular dynamics (MD) simulations to study the self-assembly procedure of a system of randomly placed lipid molecules, water beads, and a nanoparticle (NP). The self-assembly results in the formation of the nanoparticle-supported lipid bilayer (NPSLBL), with the self-assembly mechanism being driven by events such as the formation of small lipid clusters, merging of the lipid clusters in the vicinity of the NP to form NP-embedded vesicle with a pore, and collapsing of that pore to eventually form the equilibrated NPSLBL system overcoming a large free-energy barrier. Subsequently, we quantify the properties and the configurations of this NPSLBL system. We reveal that unlike our proposition of an equal number of lipid molecules occupying the inner and outer leaflets in a recent report studying the properties of a preassembled lipid bilayer, the equilibrated self-assembled NPSLBL system demonstrates a much larger number of lipid molecules occupying the outer leaflet as compared to the inner leaflet. Second, the thickness of the water layer entrapped between the NP and the inner leaflet shows similar values as predicted by experiments and our previous study. Finally, we reveal that, similar to our previous study, the diffusivity of the lipid molecules in the outer leaflet is larger than that in the inner leaflet but, due to higher temperature employed during our simulations, are even larger than that predicted by our previous study.

Ferroptosis is a type of cell death caused by the pathogenic accumulation of lipid hydroperoxides. Pharmacological mechanisms to induce ferroptosis may provide a way to kill cancer cells that are resistant to other forms of cell death like apoptosis. Nonetheless, the proteins that regulate ferroptotic sensitivity in cancer cells remain incompletely understood. Here, we screened a panel of inhibitors of serine hydrolases-an enzyme class important for regulating lipid metabolism-for potentiation of ferroptosis in HT1080 fibrosarcoma cells. We found that DO264, a selective inhibitor of the lyso- and ox-phosphatidylserine (PS) lipase ABHD12, enhances ferroptotic death caused by RSL3, an inhibitor of the lipid peroxidase GPX4. RSL3-induced ferroptosis was also potentiated by genetic disruption of ABHD12. Metabolomic experiments revealed that, in addition to elevated lyso-PS, ABHD12-inactivated cells show higher quantities of arachidonate (C20:4)-containing PS and 2-arachidonoyl glycerol, pointing to potential oxidation-sensitive lipid mediators of ferroptosis regulated by ABHD12.

Poly(3,4-ethylenedioxythiophene):poly(4-styrene sulfonate) (PEDOT:PSS) has demonstrated outstanding performance as a charge transport layer or an electrode in various electronic devices, including organic solar cells, organic light-emitting diodes, and organic field-effect transistors (OFETs). The electrical properties of these devices are affected by the contact properties at the PEDOT:PSS-semiconductor junction. In this research, we performed work function (WF) engineering of electrohydrodynamic (EHD)-jet-printed PEDOT:PSS and successfully used it as an electrode to fabricate high-performance OFETs and complementary logic circuits. Two types of PEDOT:PSS materials-one with a high WF (HWF, 5.28 eV) and the other with a low WF (LWF, 4.53 eV)-were synthesized and EHD-jet-printed. The WF of PEDOT:PSS was deterministically modulated by approximately 0.75 eV through simple mixing of the two synthesized PEDOT:PSS materials in various ratios. OFETs fabricated with HWF and LWF PEDOT:PSS electrodes showed excellent electrical properties, including the ON/OFF switching ratio higher than 10 7 and the highest carrier mobility greater than 1 cm 2 ·V -1 ·s -1 . Furthermore, the HWF and LWF PEDOT:PSS electrodes were integrated to fabricate complementary metal-oxide-semiconductor (CMOS) NOT, NOR, and NAND circuits.

During the evolution of life on earth, the emergence of lipid membrane-bounded compartments is one of the most enigmatic events. Endosymbiosis has been hypothesized as one of the solutions. In this work, using a coacervate droplet formed by single-stranded oligonucleotides (ss-oligo) and poly(l-lysine) (PLL) as the protocell model, we monitored the uptake of liposomes of different types and studied the dynamic behavior of the resulting composite droplet under the electric field. The coacervate droplet exhibits affinity for the liposomes of varying charges. However, the permeation of liposome is also controlled by electrostatic interactions. Dominated by electrostatic attraction, the positively charged liposome is retained inside the droplet as growing fibrous structures, while the negatively charged liposome is mainly coated on the droplet surface. Permeation and even distribution occur when the liposome and the droplet carry the same charges, or at least one of them is neutral. As an electric field is applied to trigger repetitive cycles of vacuolization in the ss-oligo/PLL droplet, the fibrous structure formed by the positively charged liposome is basically intact, while a new phase is generated together with uneven mass transport as the negatively charged liposome is internalized. Interestingly, the release of daughter droplets with similar components occurs on the droplet containing neutral liposomes. Our work not only provides a step toward creating protocells with hierarchical structures and biofunctions using a biogenetic material via simple mixing but also sheds light on the possible origin of the lipid structure inside a living organism.

MXenes, an emerging class of two-dimensional (2D) transition metal carbides and nitrides, have potential for application as high-performance, low-cost electrodes in organic field-effect transistors (OFETs) because of their water dispersibility, high conductivity, and work-function tunability. In this study, we successfully fabricated a large-scale, uniform Ti 3 C 2 T x MXene electrode array on a flexible plastic substrate for application in high-performance OFETs. The work function of the Ti 3 C 2 T x MXene electrodes was also effectively modulated via chemical doping with NH 3 . The fabricated OFETs with Ti 3 C 2 T x MXene electrodes exhibited excellent device performance, such as a maximum carrier mobility of ∼1 cm 2 ·V -1 ·s -1 and an on-off current ratio of ∼10 7 for both p - type and n - type OFETs, even though all the electrode and dielectric layers were fabricated on the plastic substrate by solution processing. Furthermore, MXene-electrode-based complementary logic circuits, such as NOT, NAND, and NOR, were fabricated via integration of p - type and n - type OFETs. The proposed approach is expected to expand the application range of MXenes to other OFET-based electronic devices, such as organic light-emitting displays and electronic skins.

Protein lysine fatty acylation is increasingly recognized as a prevalent and important protein post-translation modification. Recently, it has been shown that K-Ras4a, R-Ras2, and Rac1 are regulated by lysine fatty acylation. Here, we investigated whether other members of the Ras superfamily could also be regulated by lysine fatty acylation. Several small GTPases exhibit hydroxylamine resistant fatty acylation, suggesting they may also have protein lysine fatty acylation. We further characterized one of these GTPases, RalB. We show that RalB has C-terminal lysine fatty acylation, with the predominant modification site being Lys200. The lysine acylation of RalB is regulated by SIRT2, a member of the sirtuin family of nicotinamide adenine dinucleotide (NAD)-dependent protein lysine deacylases. Lysine fatty acylated RalB exhibited enhanced plasma membrane localization and recruited its known effectors Sec5 and Exo84, members of the exocyst complex, to the plasma membrane. RalB lysine fatty acylation did not affect the proliferation or anchorage-independent growth but did affect the trans-well migration of A549 lung cancer cells. This study thus identified an additional function for protein lysine fatty acylation and the deacylase SIRT2.

Black garlic is a new garlic product produced through fermentation of fresh garlic and is very popular in Asia countries due to its health benefits. Its key aroma-active compounds were characterized by gas chromatography-olfactometry-mass spectrometry (GC-O-MS), gas chromatography-time-of-flight mass spectrometry (GC-TOFMS), and sensory evaluation. In total 52 aroma compounds were identified, and 15 of them with high flavor dilution (FD) factors based on aroma extract dilution analysis (AEDA) were selected and quantitated. Finally, 9 key aroma-active compounds, including acetic acid (sour), allyl methyl trisulfide (cooked garlic), Furaneol (caramel), diallyldisulfide (garlic), diallyltrisulfide (sulfur), ( E , Z )-2,6-nonadien-1-ol (cucumber), 3-methylbutanoic acid (sweat), 5-heptyldihydro-2(3 H )-furanone (apricot), and diallyl sulfide (garlic), were determined through aroma recombination and omission experiment. In addition to the sulfur-containing compounds, heterocyclic compounds were the major aroma contributors in black garlic. Sensory evaluation revealed that the flavor profile of black garlic mainly consisted of sulfur, sour, sweet, fresh, sauce, gasoline, and roasted odors.

Construction of protocell models from prebiotically plausible components to mimic the basic features or functions of living cells is still a challenge. In this work, we prepare a hybrid protocell model by coating sodium oleate on the coacervate droplet constituted by poly(l-lysine) and oligonucleotide and investigate the transport of different molecules under electric field. Results show that sodium oleate forms a layered viscoelastic membrane on the droplet surface, which is selectively permeable to small, polar molecules, such as oligolysine. As the droplet is stimulated at 10 V cm -1 , the oleate membrane slips along the direction of electric field while maintaining its integrity. Most of the molecules are still excluded under such conditions. As repetitive cycles of vacuolization occur at 20 V cm -1 , all molecules are internalized and sequestrated in the droplet through their specific pathways except enzyme, which anchors in the oleate membrane and is immune to electric field. Cascade enzymatic reactions are then carried out, and the product generated from the membrane exhibits a time-dependent concentration gradient across the droplet. Our work makes a step toward the nonequilibrium functionalization of synthetic protocells capable of biomimetic operations.

In valvular replacement surgery, especially in the construction of bioprosthetic valves with decellularized pericardial xenograft, glutaraldehyde (GA) is routinely utilized as the golden standard reagent to fix bovine or porcine pericardial tissues. However, the apparent defects of GA, including cytotoxicity and calcification, increase the probability of leaflet failure and motivate the exploration for alternatives. Thus, the aim of this study is to develop nonglutaraldehyde combined-cross-linking reagents composed of alginate-EDC/NHS (Alg) or oxidized alginate-EDC/NHS (Alg-CHO) as substitute for GA, which is confirmed to be less toxic and more biocompatible. Evaluations of the fixed acellular bovine pericardial tissues included mechanical performance, thermodynamics/enzymatic/in vivo stability tests, blood compatibility assay, cytocompatibility assay, in vitro anticalcification, and in vivo anticalcification assay by subcutaneous implantation in juvenile Wistar rats. The data revealed that the tissues fixed with the combined cross-linking reagents were superior to GA control and commercially available Sino product in terms of better in vitro hemocompatibility and cytocompatibility, lower calcification levels, better thermodynamics stability, and better regenerative capacity in subcutaneous implants, while the mechanical strength and in vivo stability were comparable. Considering all above performances, it indicated that both Alg and Alg-CHO are appropriate to replace GA as the cross-linkers for biological tissue, particularly as a nonglutaraldehyde fixation for off the shelf decellularized bovine pericardial tissue in the anticalcification cardiac valve applications. Nevertheless, studies on the long-term durability and calcification-resistance capacity in large animal model are further needed.