High Capacity Research Articles

One-step chemical vapor deposition synthesis of Si NWs@C core/shell anodes without additional catalysts by the oxide-assisted growth mechanism for lithium-ion batteries.

Si NWs@C core/shell anodes for lithium-ion batteries were synthesized via a one-step environmental-pressure chemical vapor deposition (CVD) process utilizing nano-silicon and methane as raw materials. In this structure, the silicon nanowire core is obtained by controlling the temperature above 900 °C to catalyze the growth of nano-silicon particles coated with a natural oxide layer according to the oxide-assisted growth (OAG) mechanism, while the carbon as a protective coating shell is derived from methane cracking. In contrast to the conventional nanowire catalytic approach, this method obviates the addition of metal catalysts while ensuring a straightforward and scalable process. This Si NWs@C electrode displayed excellent electrochemical performance, exhibiting high reversible capacity (745.8 mA h g-1) and excellent cycling stability (91.3% after 100 cycles at 0.5 A g-1).

High-Entropy Prussian Blue Analogues Enable Lattice Respiration for Ultra-Stable Aqueous Aluminum-Ion Batteries.

Aqueous aluminum ion batteries (AAIBs) hold significant potential for grid-scale energy storage owing to their intrinsic safety, high theoretical capacity, and abundance of aluminum. However, the strong electrostatic interactions and delayed charge compensation between high-charge-density aluminum ions and the fixed lattice in conventional cathodes impede the development of high-performance AAIBs. To address this issue, we introduce, for the first time, high-entropy Prussian blue analogs (HEPBAs) as cathodes in AAIBs with unique lattice tolerance and efficient multipath electron transfer. Benefiting from the intrinsic long-range disorder and robust lattice strain field, HEPBAs enable the manifestation of the lattice respiration effect and minimize lattice volume changes, thereby achieving one of the best long-term stabilities (91.2% capacity retention after 10,000 cycles at 5.0 A g-1) in AAIBs. Additionally, the interaction between the diverse metal atoms generates a broadened d-band and reduced degeneracy compared with conventional PBAs, which enhances the electron transfer efficiency with one of the best rate performance (79.2 mAh g-1 at 5.0 A g-1) in AAIBs. Furthermore, exceptional element selectivity in HEPBAs with unique cocktail effect could facile tune electrochemical behavior. Overall, the newly developed HEPBAs with a high-entropy effect exhibit promising solutions for advancing AAIBs and multivalent-ion batteries. This article is protected by copyright. All rights reserved.

First principles investigation of Li[formula omitted]Si and Li[formula omitted]Sn alloys: Unraveling atomic-scale influences on material properties

Commercial batteries have currently reached their peak specific capacity, which proves insufficient for the ongoing global energy transition. Consequently, there has been a surge of interest in developing new materials over the last decade, especially those based on silicon (Si) and tin (Sn), known for their high capacity. Despite numerous publications highlighting the advantages of these materials, crucial questions remain regarding volume expansion that must be addressed to propose effective solutions and facilitate their widespread commercial application. In this study, density functional theory was employed to investigate the formation of LixM (M = Si, Sn). Our analysis delves into crystal (c-LixM), amorphous (a-LixM), and amorphous slab (s-LixM) configurations during structural optimization calculations, with the aim of comparing and contrasting relevant findings. The exploration encompasses energetic aspects, volume expansion, and electronic properties. The obtained data enables the simulation of lithiation potential curves for each structural type, directly comparable with experimental results of these materials functioning as anodes in lithium-ion batteries. Notably, the volume expansion of a-LixM exhibits non-linear behavior, correlating with characteristic plateaus in the voltage profile curves.

Vacancy-Defect Ternary Topological Insulators Bi2Se2Te Encapsulated in Mesoporous Carbon Spheres for High Performance Sodium Ion Batteries and Hybrid Capacitors.

Ternary topological insulators have attracted worldwide attention because of their broad application prospects in fields such as magnetism, optics, electronics, and quantum computing. However, their potential and electrochemical mechanisms in sodium ion batteries (SIBs) and hybrid capacitors (SIHCs) have not been fully studied. Herein, a composite material comprising vacancy-defects ternary topological insulator Bi2Se2Te encapsulated in mesoporous carbon spheres (Bi2Se2Te@C) is designed. Bi2Se2Te with ample vacancy-defects has a wide interlayer spacing to enable frequent insertion/extraction of Na+ and boost reaction kinetics within the electrode. Meanwhile, the Bi2Se2Te@C with optimized yolk-shell structure can buffer the volume variation without breaking the outer protective carbon shell, ensuring structural stability and integrity. As expected, the Bi2Se2Te@C electrode delivers high reversible capacity and excellent rate capability in half SIB cells. Various electrochemical analyses and theoretical calculations manifest that Bi2Se2Te@C anode confirms the synergistic effect of ternary chalcogenide systems and suitable void space yolk-shell structure. Consequently, the full cells of SIB and SIHC coupled with Bi2Se2Te@C anode exhibit good performance and high energy/power density, indicating its widespread practical applications. This design is expected to offer a reliable strategy for further exploring advanced topological insulators in Na+-based storage systems.

Ab Initio Design of Ni‐Rich Cathode Material with Assistance of Machine Learning for High Energy Lithium‐Ion Batteries

With the widespread use of lithium‐ion batteries in electric vehicles, energy storage, and mobile terminals, there is an urgent need to develop cathode materials with specific properties. However, existing material control synthesis routes based on repetitive experiments are often costly and inefficient, which is unsuitable for the broader application of novel materials. The development of machine learning and its combination with materials design offers a potential pathway for optimizing materials. Here, we present a design synthesis paradigm for developing high energy Ni‐rich cathodes with thermal/kinetic simulation and propose a coupled image‐morphology machine learning model. The paradigm can accurately predict the reaction conditions required for synthesizing cathode precursors with specific morphologies, helping to shorten the experimental duration and costs. After the model‐guided design synthesis, cathode materials with different morphological characteristics can be obtained, and the best shows a high discharge capacity of 206 mAh g−1 at 0.1C and 83% capacity retention after 200 cycles. This work provides guidance for designing cathode materials for lithium‐ion batteries, which may point the way to a fast and cost‐effective direction for controlling the morphology of all types of particles.

Self‐Supporting Solid Electrolyte Based on Supramolecular Interaction for Stable Li Metal Batteries

Li metal batteries based on solid polymer electrolytes offer the benefits of high energy density and safety, as well as extended cycling life, making them an excellent candidate for the next‐generation battery system. However, current solid polymer electrolytes still suffer from low ion conductivity and Li+ transfer number, which seriously restricts its practical application. Herein, a self‐supporting composite solid polymer electrolyte was prepared, where phenolic resin rich in hydroxyl groups (BR) and polyethylene oxide (PEO) are mixed evenly and poured onto a cellulose membrane in one step. In such an electrolyte, PEO and BR combine to form intermolecular hydrogen bonds, lowering the crystallinity of PEO and increasing the Li+ transfer number. Lastly, the obtained solid electrolytes exhibited a high ion conductivity (1.1×10‐4 S cm‐1) and Li+ transfer number (0.53), as well as improved electrochemical window. Consequently, Li || Li symmetrical cells can run stably for more than 700 h at 0.1 mA cm‐2/0.25 mAh cm‐2. And full cells with LiFePO4 cathode can also demonstrate high discharge capacity of 152.12 mAh g‐1 and rate performance. We believe that such a design based on supramolecular interaction offer a new avenue to advanced solid polymer electrolytes.

Preparation of surface molecularly‐imprinted magnetic kaolin for selective separation and determination of thiabendazole

AbstractIn this study, a selective sorbent was fabricated by combining a surface molecularly‐imprinted polymer and magnetic kaolin for reliable quantification of thiabendazole (TBZ) coupled with spectrofluorimetry. Several surface characterization methods were conducted to confirm the synthesis of TBZ‐imprinted magnetic kaolin with a polymer thickness of ~48 nm. The molecularly‐imprinted magnetic kaolin (MIP@MKLN) showed high adsorption capacity (8.7 mg/g), remarkable selectivity with an imprinting factor of 3.71 and excellent regeneration ability for up to 10 uses without significant change of its initial adsorption capacity for TBZ. The proposed method had linear range from 5 to 500 μg/mL TBZ concentration with a correlation coefficient of 0.995 and the limit of detection was 1.4 μg/mL. MIP@MKLN was used for selective separation and quantification of TBZ in orange and lemon samples. There were high recovery values ranging from 96.4% to 100.2% with lower relative standard deviations (less than 5%) in the spiked samples under optimized conditions. Overall, the proposed method based on MIP@MKLN as an excellent sorbent could produce a feasible, convenient, and promising method for rapid, selective, and sensitive quantification of TBZ in real samples.

Engineering Oxygen Vacancies in In2O3 with Enhanced Polysulfides Immobilization and Selective Catalytic Capability.

Lithium-sulfur (Li-S) battery is identified as an ideal candidate for next-generation energy storage systems in consideration of its high theoretical energy density and abundant sulfur resources. However, the shuttling behavior of soluble polysulfides (LiPSs) and their sluggish reaction kinetics severely limit the practical application of the current Li-S battery. In this work, a series of In2O3 nanocubes with different oxygen vacancy concentrations are designed and prepared via a facile self-template method. The introduced oxygen vacancy on In2O3 can effectively rearrange the charge distribution and enhance sulfiphilic property. Moreover, the In2O3 with high oxygen vacancy concentration (H-In2O3) can slightly slow down the solid-liquid conversion process and significantly accelerate the liquid-solid conversion process, thus reducing the accumulation of LiPSs in electrolyte and inhibiting the shuttle effect. Contributed by the unique selective catalytic capability, the prepared H-In2O3 exhibits excellent electrochemical performance when used as sulfur host. For instance, a high reversible capacity of 609 mAh g-1 is obtained with only 0.044% capacity decay per cycle over 1000 cycles at 1.0C. This work presents a typical example for designing advanced sulfur hosts, which is crucial for the commercialization of Li-S battery.

Scalable Synthesis of SiOx-TiON Composite As an Ultrastable Anode for Li-Ion Half/Full Batteries.

Among various anode materials, SiOx is regarded as the next generation of promising anode due to its advantages of high theoretical capacity with 2680 mA h g-1, low lithium voltage platform, and rich natural resources. However, the pure SiOx-based materials have slow lithium storage kinetics attributed to their low electron/ion conductive properties and the large volume change during lithiation/delithiation, restricting their practical application. Optimizing the SiOx material structures and the fabricating methods to mitigate these fatal defects and adapt to the market demand for energy density is critical. Hence, SiOx material with TiO1-xNx phase modification has been prepared by simple, low-cost, and scalable ball milling and then combined with nitridation. Consequently, based on the TiO1-xNx modified layer, which boosts high ionic/electronic conductivity, chemical stability, and excellent mechanical properties, the SiOx@TON-10 electrode shows highly stable lithium-ion storage performance for lithium-ion half/full batteries due to a stable solid-electrolyte interface layer, fast Li+ transport channel, and alleviative volumetric expansion, further verifying its practical feasibility and universal applicability.

Regulation of cerebral blood flow boosts precise brain targeting of vinpocetine-derived ionizable-lipidoid nanoparticles

Despite advances in active drug targeting for blood-brain barrier penetration, two key challenges persist: first, attachment of a targeting ligand to the drug or drug carrier does not enhance its brain biodistribution; and second, many brain diseases are intricately linked to microcirculation disorders that significantly impede drug accumulation within brain lesions even after they cross the barrier. Inspired by the neuroprotective properties of vinpocetine, which regulates cerebral blood flow, we propose a molecular library design centered on this class of cyclic tertiary amine compounds and develop a self-enhanced brain-targeted nucleic acid delivery system. Our findings reveal that: (i) vinpocetine-derived ionizable-lipidoid nanoparticles efficiently breach the blood-brain barrier; (ii) they have high gene-loading capacity, facilitating endosomal escape and intracellular transport; (iii) their administration is safe with minimal immunogenicity even with prolonged use; and (iv) they have potent pharmacologic brain-protective activity and may synergize with treatments for brain disorders as demonstrated in male APP/PS1 mice.

Antioxidant Interfaces Enabled by Self‐Deoxidizing and Self‐Dehydrogenating Redox Couple for Reversible Zinc Metal Batteries

AbstractParasitic electrolyte reactions and dendrite growth make Zn metal anodes with high Zn utilization rates (ZURs) more inaccessible, holding back the advance of aqueous zinc metal batteries (AZMBs). Here, sodium isoascorbate (SIA) is introduced to aqueous electrolytes as a self‐deoxidizing and self‐dehydrogenating additive. Coexisting C6H7O6−/C6H5O6− couple spontaneously captures dissolved oxygen and eliminates generated hydrogen by acting as a redox buffer, which leads to the creation of antioxidant Interfaces due to an in situ formed ZnCO3‐dominated solid electrolyte interphase (SEI). This SEI enables the (100) faceted electrode with dendrite‐free and non‐corrosive Zn plating/stripping, thus yielding a Coulombic efficiency of 99.7% up to 1100 h at 5 mAh cm−2, as well as a stable cycle sustaining for over 335 h under a high ZUR of 85.5%. Full‐cell properties are demonstrated by matching a poly(3,4‐ethylenedioxythiophene) intercalated vanadium oxide (PEDOT‐V2O5) cathode, which harvests a high capacity of 302 mAh g−1 (at 0.01 A g−1) and holds 94.2% capacity retention over 600 cycles (at 1 A g−1) under practical conditions (N/P = 4.2 and E/C = 7.6 µL mg−1). These findings provide a new solution for electrolyte design for industrializing AZMBs.

Electropolymerization of a Carbonyl-Modified Dihydropyrazine Derivative for Aqueous Zinc Batteries with Ultrahigh Cycling Stability.

The design of aqueous zinc-ion batteries (ZIBs) that have high specific capacity and long-term stability is essential for future large-scale energy storage systems. Cathode materials with extended π-conjugation and abundant active sites are desirable to enhance the charge storage performance and the cycling stability of the aqueous ZIB. Based on this concept, 6,9-dihydropyrazino[2,3-g]quinoxaline-2,3,7,8(1H,4H)-tetrone was chosen as the monomer to be electropolymerized onto carbon cloth (PDHPQ-Tetrone/CC). When used as the cathode material for aqueous ZIBs, an exceptional cycling life (>20,000 cycles) at a current density of 10 A g-1 was achieved, with the specific capacity maintained at 82.8% and with the Coulombic efficiency at around 100% throughout cycling. At the charge-discharge current density of 0.1 A g-1, the ZIB with PDHPQ-Tetrone/CC achieved a high specific capacity of 248 mAh g-1. Kinetic analyses showed that both surface-capacitive-controlled processes and semi-infinite diffusion-controlled processes contribute to the stored charge. The charge storage mechanism was investigated with ex situ characterizations and involves the redox processes of carbonyl/hydroxyl and amino/imino groups coupled with insertion and extraction of both Zn2+ and H+.

The synergistic impact of Universal Health Coverage and Global Health Security on health service delivery during the Coronavirus Disease-19 pandemic: A difference-in-difference study of childhood immunization coverage from 192 countries.

Universal Health Coverage (UHC) and Global Health Security (GHS) are two high-priority global health agendas that seek to foster health system resilience against health emergencies. Many countries have had to prioritize one agenda over the other due to scarce resources and political pressures. To aid policymakers' decision-making, this study investigated the individual and synergistic effects of countries' UHC and GHS capacities in safeguarding essential health service delivery during the COVID-19 pandemic. We used a quasi-experimental difference-in-difference methodology to quantify the relationship between 192 countries' progress towards UHC and GHS and those countries' abilities to provide 12 essential childhood immunization services between 2015 and 2021. We used the 2019 UHC Service Coverage Index (SCI) to divide countries into a "high UHC group" (UHC SCI≥75) and the rest (UHC SCI 75), and similarly used the 2019 GHS Index (GHSI) to divide countries into a "high GHS group" (GHSI≥65) and the rest (GHSI<65). All analyses were adjusted for potential confounders. Countries with high UHC scores prevented a 1.14% (95% CI: 0.39%, 1.90%) reduction in immunization coverage across 2020 and 2021 whereas countries with high GHSI scores prevented a 1.10% (95% CI: 0.57%, 1.63%) reduction in immunization coverage over the same time period. The stratified DiD models showed that across both years, high UHC capacity needed to be augmented with high GHS capacity to prevent a decline in immunization coverage while high GHS alone was able to safeguard immunization coverage. This study found that greater progress towards both UHC and GHS capacities safeguarded essential health service delivery during the pandemic but only progress towards GHS capacity was both a necessary and likely sufficient element for yielding this protective effect. Our results call for strategic investments into both health agendas and future research into possible synergistic effects of the two health agendas.

Freestanding Ammonium Vanadate Composite Cathodes with Lattice Self-Regulation and Ion Exchange for Long-Lasting Ca-Ion Batteries.

Calcium-ion batteries (CIBs) have emerged as a promising alternative for electrochemical energy storage. The lack of high-performance cathode materials severely limits the development of CIBs. Vanadium oxides are particularly attractive as cathode materials for CIBs, and preinsertion chemistry is often used to improve their calcium storage performance. However, the room temperature cycling lifespan of vanadium oxides in organic electrolytes still falls short of 1000 cycles. Here, based on preinsertion chemistry, the cycling life of vanadium oxides is further improved by integrated electrode and electrolyte engineering. Utilizing a tailored Ca electrolyte, the constructed freestanding (NH4)2V6O16·1.35H2O@graphene oxide@carbon nanotube (NHVO-H@GO@CNT) composite cathode achieves a 305 mAh g-1 high capacity and 10000 cycles record-long life. Additionally, for the first time, a Ca-ion hybrid capacitor full cell is assembled and delivers a capacity of 62.8 mAh g-1. The calcium storage mechanism of NHVO-H@GO@CNT based on a two-phase reaction and the exchange of NH4 + and Ca2+ during cycling are revealed. The lattice self-regulation of V─O layers is observed and the layered vanadium oxides with Ca2+ pillars formed by ion exchange exhibit higher capacity. This work provides novel strategies to enhance the calcium storage performance of vanadium oxides via integrated structural design of electrodes and electrolyte modification.

UHVDC transmission line diagnosis method for integrated community energy system based on wavelet analysis

With the large-scale development of renewable energy power, China has faced with the challenges of the reverse regional distribution of wind and solar resources and power load, as well as the intermittency and randomness of renewable energy power. Therefore, China is vigorously developing ultra-high voltage direct current (UHVDC) transmission technology to solve the problem of insufficient flexibility caused by the uncertainty of renewable energy and the fluctuation of multi-energy loads in integrated community energy systems. UHVDC plays an increasingly pivotal role in the west-east transmission system in China’s power system due to its high transmission capacity and long transmission distance. Once the fault occurs in the ultra-high voltage direct (UHVD) transmission line, quick and accurate fault location identification is of great significance. Hence, this paper proposes a UHVDC transmission line diagnosis method based on wavelet analysis for integrated community energy systems. Wavelet transform (WT) is used to decompose the transient signal on a multi-scale, and then power systems computer-aided design (PSCAD) software is utilized for simulation calculation to obtain the singular spectrum entropy of each layer and facilitate wavelet transformations for signal denoising with advanced tools such as MATLAB. The prediction results can distinguish outside the rectification side fault, within the rectification side fault, and outside the inverter fault with an accuracy of 100%. A large number of simulations demonstrate that combining singular spectrum entropy with support vector machines (SVM) has emerged as a robust technique for integrated community energy systems, suggesting its potential as a standard method in UHVDC transmission line diagnosis. This study is of significant reference for realizing the complementarity of multiple types of power supply and ensuring a reliable power supply.

High loading electrode with superior electron/ion transport network for high performance lithium-ion batteries

High loading electrode design is beneficial to increase the energy density of lithium ion batteries. Two obstacles for the high loading electrode application should be removed, including the limitation on ion/electron transport within high loading electrode and the structure stability. Here, the electron conduction on LiNi0.8Co0.1Mn0.1O2 cathodes is enhanced with evenly and tightly Ketjen Black coating via high-speed dry mixing, while carbon nanotube is added to enhance the electron conduction between LiNi0.8Co0.1Mn0.1O2 particles, thus to construct three-dimensional electron migration channel. In addition, the large amount of electrolyte adsorbed by porous Ketjen Black and carbon nanotube enhances the Li+ ion diffusivity in this network. As a result, LiNi0.8Co0.1Mn0.1O2 electrode with only 1 % Ketjen Black and 3 % carbon nanotube can achieve both high electron/Li+ ion diffusivity and high parking density (2.2 g cm−3). A thick electrode with an areal mass loading of 20 mg cm−2 shows a high specific capacity of 111.2 mA h g−1 at 4 C and capacity retention rate of 98.2 % after 100 cycles at 2 C.

Production of Anthocyanin-Rich Red Rose Petal Extract by Enzymatic Maceration

The use of enzymes to hydrolyze the plant cell matrix is a method known for extracting bioactive substances. The current work used this strategy to produce a rose petal extract rich in anthocyanins that is stable in the presence of marine polysaccharides and has a high antioxidant activity. The process evaluation was carried out sequentially, initially comparing water, ethanol, and their mixtures to anthocyanins extracted in the presence or absence of enzymes. Then, a multi-objective desirability function optimized experimental conditions such as solvent and enzyme concentrations. This study is the first report describing the use of a statistical tool, the central composite rotatable design (CCRD), to optimize anthocyanin extraction from rose petals. This method obtained a maximum extraction of 9.99 mg/g of phenols. The stability of the rose petal extract when using marine polysaccharides retained 60% of the anthocyanins over 28 days without deterioration when protected from sunlight but was practically degraded upon exposure to sunlight. The rose petal extract demonstrated a very high antioxidant capacity of 3.19 μg/mL, close to the literature data for citrus compounds, known to be high in antioxidant compounds for cosmetic food purposes.

Stabilizing High-Voltage Performance of Nickel-Rich Cathodes via Facile Solvothermally Synthesized Niobium-Doped Strontium Titanate.

Ni-rich layered ternary cathodes are promising candidates thanks to their low toxic Co-content and high energy density (∼800 Wh/kg). However, a critical challenge in developing Ni-rich cathodes is to improve cyclic stability, especially under high voltage (>4.3 V), which directly affects the performance and lifespan of the battery. In this study, niobium-doped strontium titanate (Nb-STO) is successfully synthesized via a facile solvothermal method and used as a surface modification layer onto the LiNi0.8Co0.1Mn0.1O2 (NCM811) cathode. The results exhibited that the Nb-STO modification significantly improved the cycling stability of the cathode material even under high-voltage (4.5 V) operational conditions. In particular, the best sample in our work could provide a high discharge capacity of ∼190 mAh/g after 100 cycles under 1 C with capacity retention over 84% in the voltage range of 3.0-4.5 V, superior to the pristine NCM811 (∼61%) and pure STO modified STO-811-600 (∼76%) samples under the same conditions. The improved electrochemical performance and stability of NCM811 under high voltage should be attributed to not only preventing the dissolution of the transition metals, further reducing the electrolyte's degradation by the end of charge, but also alleviating the internal resistance growth from uncontrollable cathode-electrolyte interface (CEI) evolution. These findings suggest that the as-synthesized STO with an optimized Nb-doping ratio could be a promising candidate for stabilizing Ni-rich cathode materials to facilitate the widespread commercialization of Ni-rich cathodes in modern LIBs.

Multifunctional 2D hemin-bridged MOF for the efficient removal and dual-mode detection of organophosphorus pesticides.

The high-residual and bioaccumulation property of organophosphorus pesticides (OPs) creates enormous risks towards the ecological environment and human health, promoting the research for smart adsorbents and detection methods. Herein, 2D hemin-bridged MOF nanozyme (2D-ZHM) was fabricated and applied tothe efficient removal and ultrasensitive dual-mode aptasensing of OPs. On the one hand, the prepared 2D-ZHM contained Zr-OH groups with high affinity for phosphate groups, endowing it with selective recognition and high adsorption capacity for OPs (285.7mgg-1 for glyphosate). On the other hand, the enhanced peroxidase-mimicking biocatalytic property of 2D-ZHM allowed rapid H2O2-directed transformation of 3,3',5,5'-tetramethylbenzidine to oxidic product, producing detectable colorimetric or photothermal signals. Using aptamers of specific recognition capacity, the rapid quantification of two typical OPs, glyphosate and omethoate, was realized with remarkable sensitivity and selectivity. The limit of detections (LODs) of glyphosate were 0.004nM and 0.02nM for colorimetric and photothermal methods, respectively, and the LODs of omethoate were 0.005nM and 0.04nM for colorimetric and photothermal methods, respectively. Theconstructed dual-mode aptasensing platform exhibited outstanding performance for monitoring OPs in water and fruit samples. This work provides a novel pathway to develop MOF-based artificial peroxidase and integrated platform for pollutant removal and multi-mode aptasensing.

CO2-Based Stable Porous Metal-Organic Frameworks for CO2 Utilization.

The transformation of carbon dioxide (CO2) into functional materials has garnered considerable worldwide interest. Metal-organic frameworks (MOFs), as a distinctive class of materials, have made great contributions to CO2 capture and conversion. However, facile conversion of CO2 to stable porous MOFs for CO2 utilization remains unexplored. Herein, we present a facile methodology of using CO2 to synthesize stable zirconium-based MOFs. Two zirconium-based MOFs CO2-Zr-DEP and CO2-Zr-DEDP with face-centered cubic topology were obtained via a sequential desilylation-carboxylation-coordination reaction. The MOFs exhibit excellent crystallinity, as verified through powder X-ray diffraction and high-resolution transmission electron microscopy analyses. They also have notable porosity with high surface area (SBET up to 3688 m2 g-1) and good CO2 adsorption capacity (up to 12.5 wt %). The resulting MOFs have abundant alkyne functional moieties, confirmed through 13C cross-polarization/magic angle spinning nuclear magnetic resonance and Fourier transform infrared spectra. Leveraging the catalytic prowess of Ag(I) in diverse CO2-involved reactions, we incorporated Ag(I) into zirconium-based MOFs, capitalizing on their interactions with carbon-carbon π-bonds of alkynes, thereby forming a heterogeneous catalyst. This catalyst demonstrates outstanding efficiency in catalyzing the conversion of CO2 and propargylic alcohols into cyclic carbonates, achieving >99% yield at room temperature and atmospheric pressure conditions. Thus, this work provides a dual CO2 utilization strategy, encompassing the synthesis of CO2-based MOFs (20-24 wt % from CO2) and their subsequent application in CO2 capture and conversion processes. This approach significantly enhances overall CO2 utilization.