J Am Chem Soc
August 2025
The development of adsorbents for ammonia capture and separation is a challenging task, with significant industrial relevance. We report herein, for the first time, open aluminophosphate frameworks for on-demand ammonia adsorption. Under ambient conditions, the AlPO-18 molecular sieve exhibits exceptional dynamic ammonia uptake of 3.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
May 2025
Ethylene dimerization is a crucial chemical process, which currently relies on organo-metallic catalysis with the assistance of overdosed additives as cocatalysts. Heterogeneous nickel catalysts have been investigated as alternatives for ethylene dimerization, however suffer from low catalytic activity and/or poor 1-butene selectivity. Herein, we report a simple two-step ion-exchange strategy for the preparation of Ni-Mg-Y zeolite containing well-defined coordinatively-unsaturated nickel centers as a promising catalyst for ethylene dimerization.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
February 2025
The adsorptive separation of molecules with very similar physical properties is always a challenging task. Reported herein is the design and tailoring of zeolite adsorbent for the precise discrimination and separation of CO-CH mixture through the pronounced trapdoor effect. Typically, Sr exchanged K-type clinoptilolite, namely Sr/K-HEU, is developed as a robust zeolite adsorbent for inverse CO-CH separation, showing the-state-of-the-art dynamic CO/CH selectivity of 48.
View Article and Find Full Text PDFNanoscale
November 2024
Self-pillared pentasil (SPP) zeolites have received considerable interest due to their distinctive intergrowth structure, while the precise process and mechanism for the formation of SPP zeolites remain obscure. Herein, SPP zeolites (ZSM-5) have been successfully synthesized by pre-aging an Al-rich gel without employing any organic templates or seeds for the first time. The as-synthesized SPP zeolites possess a notably high external surface area while the micropores for Ar adsorption are partially blocked by excess Na, which can be fully recovered by Mg or H exchange.
View Article and Find Full Text PDFNatl Sci Rev
November 2024
J Am Chem Soc
October 2024
The selective oxidation of olefins by molecular oxygen holds great importance in the chemical industry due to its remarkable adaptability in constructing carbonyl compounds. Classical homogeneous Wacker oxidation with a complex system of PdCl-CuCl-HO is currently employed in the industrial production of acetaldehyde, which suffers from several key drawbacks. The development of alternative heterogeneous catalytic systems for Wacker-type oxidations has been hotly pursued for decades.
View Article and Find Full Text PDFChem Asian J
December 2024
The selective hydrogenation of nitroaromatics plays an essential role in the chemical industry for the synthesis of anilines and their derivatives, which are known as crucial fine chemicals and pharmaceuticals. In this study, we demonstrate the preparation of Pd/Ti monolith catalyst containing well-isolated metallic Pd sites on Ti substrate through a simple impregnation method, showing remarkable catalytic properties in the selective hydrogenation of nitroaromatics containing various functional groups. Kinetic analyses reveal an apparent activation energy of 61 kJ/mol and the kinetic isotope effect (K/K) of ~1.
View Article and Find Full Text PDFJ Am Chem Soc
March 2024
The inherent inertness and striking physicochemical similarities of krypton and xenon pose significant challenges to their separation. Reported herein is the efficient xenon capture and xenon/krypton adsorptive separation by transition metal-free zeolites under ambient conditions. The polarized environment of zeolite, denoted as local polarity, can be tuned by changing the topology, framework composition, and counter-cations, which in turn correlates with the guest-host interaction and separation performance.
View Article and Find Full Text PDFNatl Sci Rev
July 2023
The selective hydrogenation of CO to methanol by renewable hydrogen source represents an attractive route for CO recycling and is carbon neutral. Stable catalysts with high activity and methanol selectivity are being vigorously pursued, and current debates on the active site and reaction pathway need to be clarified. Here, we report a design of faujasite-encaged mononuclear Cu centers, namely Cu@FAU, for this challenging reaction.
View Article and Find Full Text PDFDalton Trans
July 2023
Efficient synthesis of zeolites with different topologies is of great significance for both fundamental research and industrial application. Herein, the SSZ-23 zeolite, an odd zeolite containing 7-membered ring (7-MR) and 9-MR channels, has been synthesized under fluorine-free conditions the route of pre-aging and pH regulation. By this novel synthesis route, the crystallization time can be significantly shortened to 3 days, nearly half as that by the conventional route in fluoride media.
View Article and Find Full Text PDFExtraframework transition metal ions (TMIs) in zeolites can serve as active sites for adsorption and catalysis. However, due to the complexity and mobility of extraframework cation sites, their applications are significantly limited and the structure-performance relationship is poorly understood. In this Perspective, stable and uniform TMIs in zeolites are exemplified and their characteristics are discussed.
View Article and Find Full Text PDFOlefin selectivity and catalyst lifetime are two key metrics for industrial methanol-to-olefin catalysts. Currently, it is very difficult to obtain high olefin selectivity and long catalyst lifetime at the same time. Herein, a feasible strategy combining precoking and steaming to directionally construct the active naphthalenic species within the crystal center of the SAPO-34 catalyst has been developed, which can not only promote the lower olefin selectivity to ∼89% (ethylene and propylene) but also prolong the catalyst lifetime by ∼3.
View Article and Find Full Text PDFBMC Public Health
September 2022
Background: To assess the interaction of sleep duration and depression on the risk of cardiovascular disease (CVD).
Methods: A total of 13,488 eligible participants were enrolled in this retrospective cohort study eventually. Baseline characteristics were extracted from the China Health and Retirement Longitudinal Study (CHARLS) database, including age, sex, diabetes, high-density lipoprotein (HDL), blood glucose (GLU), glycosylated hemoglobin (GHB) etc.
Chemistry
September 2022
The development of cost-effective sorbents for direct capture of trace CO (<1 %) from the atmosphere is an important and challenging task. Natural or commercial zeolites are promising sorbents, but their performance in adsorption of trace CO has been poorly explored to date. A systematic study on capture of trace CO by commercial faujasite zeolites reveals that the extra-framework cations play a key role on their performance.
View Article and Find Full Text PDFACS Appl Mater Interfaces
March 2022
Zeolites with good acid site accessibility and high diffusion rates are highly desirable catalysts, especially when dealing with bulk molecules. In this work, ZSM-5 zeolites with similar Si/Al ratios but different thicknesses along the -axis (from ∼30 nm to ∼5 μm), namely, two plate-like ZSM-5 zeolites and two reference zeolites have been prepared and the impacts of -axis thickness on the surface properties and catalytic cracking performances are explored. Comprehensive physiochemical studies demonstrate that reducing the -axis thickness of the zeolite crystals endows the samples with better acid site accessibility and more external surface acid sites.
View Article and Find Full Text PDFJ Am Chem Soc
March 2022
Direct propylene epoxidation with molecular oxygen is a dream reaction with 100% atom economy, but aerobic epoxidation is challenging because of the undesired over-oxidation and isomerization of epoxide products. Herein, we report the construction of uniform cobalt ions confined in faujasite zeolite, namely, Co@Y, which exhibits unprecedented catalytic performance in the aerobic epoxidation of propylene. Propylene conversion of 24.
View Article and Find Full Text PDFJ Am Chem Soc
December 2021
Understanding the unique behaviors of atomically dispersed catalysts and the origin thereof is a challenging topic. Herein, we demonstrate a facile strategy to encapsulate Pt species within Y zeolite and reveal the nature of selective hydrogenation over a Pt@Y model catalyst. The unique configuration of Pt@Y, namely atomically dispersed Pt stabilized by the surrounding oxygen atoms of six-membered rings shared by sodalite cages and supercages, enables the exclusive heterolytic activation of dihydrogen over Pt···O units, resembling the well-known classical Lewis pairs.
View Article and Find Full Text PDFIEEE J Biomed Health Inform
May 2022
The digitization of Electronic Medical Record (EMR) provides potential access to a wealth of medical information, but also presents new challenges in privacy-preserved EMR exchanging and sharing. In this paper, we propose a blockchain-based smart healthcare system with fine-grained privacy protection for reliable data exchanging and sharing among different users. We design a blockchain-enabled dynamic access control framework combined with Local Differential Privacy (LDP) strategies to provide the attribute-based privacy protection in transaction workflow.
View Article and Find Full Text PDFUnderstanding the complete reaction network and mechanism of methanol-to-hydrocarbons remains a key challenge in the field of zeolite catalysis and C1 chemistry. Inspired by the identification of the reactive surface methoxy species on solid acids, several direct mechanisms associated with the formation of the first C-C bond in methanol conversion have been recently disclosed. Identifying the stepwise involvement of the initial intermediates containing the first C-C bond in the whole reaction process of methanol-to-hydrocarbons conversion becomes possible and attractive for the further development of this important reaction.
View Article and Find Full Text PDFAs a commercial MTO catalyst, SAPO-34 zeolite exhibits excellent recyclability probably due to its intrinsic good hydrothermal stability. However, the structural dynamic changes of SAPO-34 catalyst induced by hydrocarbon pool (HP) species and the water formed during the MTO conversion as well as its long-term stability after continuous regenerations are rarely investigated and poorly understood. Herein, the dynamic changes of SAPO-34 framework during the MTO conversion were identified by 1D Al, P MAS NMR, and 2D P-Al HETCOR NMR spectroscopy.
View Article and Find Full Text PDFHistol Histopathol
November 2021
Background: Herein, we aimed to determine whether DAPK1 and its post-transcriptional regulator miR-361 were implicated in high glucose (HG)-induced podocyte injury and renal damage in db/db mice.
Materials And Methods: Podocytes were incubated with normal glucose (NG; 5 mM) or HG (30 mM). Podocyte apoptosis was evaluated using TUNEL staining.
ConspectusZeolites, accompanied by their initial discovery as natural mines and the subsequent large-scale commercial production, have played indispensable roles in various fields such as petroleum refining and the chemical industry. Understanding the characteristics of zeolites, in contrast to their counterparts with similar chemical compositions and the origin thereof, is always a hot and challenging topic. Zeolites are known as intrinsic confined systems with ordered channels on the molecular scale, and structural confinement has been proposed to explain the unique chemical behaviors of zeolites.
View Article and Find Full Text PDFObjective: Acute respiratory distress syndrome (ARDS) is defined as the acute onset of noncardiogenic edema and subsequent gas-exchange impairment due to a severe inflammatory process known as cytokine storm. Xuebijing injection (hereinafter referred to as Xuebijing) is a patent drug that was used to treat ARDS or severe pneumonia (SP) in China. However, its efficacy and mechanism of actions remain unclear.
View Article and Find Full Text PDFZeolite crystals offering a short diffusion pathway through the pore network are highly desired for a number of catalytic and molecule separation applications. Herein, we develop a simple synthetic strategy toward reducing the thickness along the axis of MFI-type crystals, thus providing a short diffusion path along the straight channel. Our approach combines preliminary aging and a fluoride-assisted low-temperature crystallization.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
March 2021