Browse
Submit Data
Databases
API
Help

Dataset Information

23 Views

0 Connections

0 Citations

0 Reanalyses

0 Downloads

Omics score: 0

One-pot construction of nitrogen-rich polymeric ionic porous networks for effective CO₂ capture and fixation.

ABSTRACT: Facile preparation of ionic porous networks (IPNs) with large and permanent porosity is highly desirable for CO₂ capture and transformation but remains a challenge. Here we report a one-pot base-mediated construction of nitrogen-rich IPNs through a combination of nucleophilic substitution and quaternisation chemistry from H-imidazole. This strategy, as proven by the model reactions of 1H-imidazole or 1-methyl-1H-imidazole with cyanuric chloride, allows for fine regulation of porosity and physicochemical properties, leading to nitrogen-rich IPNs featuring abundant ionic units and radicals. The as-prepared networks, termed IPN-CSUs, efficiently capture CO₂ (80.1 cc g^-1 at 273 K/1 bar) with an ideal CO₂/N₂ selectivity of 139.7. They can also effectively catalyse the cycloaddition reaction between CO₂ and epoxides with high yields of up to 99% under mild conditions (0.1 MPa, 298 K), suggesting their possible applications in the fields of both selective molecular separation and conversion. Unlike the previously known strategies generally involving single coupling chemistry, our strategy combining two coupling routes in one pot appears to be unique and potentially applicable to other building blocks.

SUBMITTER: Ai C

PROVIDER: S-EPMC8689585 | biostudies-literature |

REPOSITORIES: biostudies-literature

ACCESS DATA

Json Xml

Similar Datasets

One-Pot Synthesis of N-Rich Porous Carbon for Efficient CO2 Adsorption Performance.

Project description:N-enriched porous carbons have played an important part in CO2 adsorption application thanks to their abundant porosity, high stability and tailorable surface properties while still suffering from a non-efficient and high-cost synthesis method. Herein, a series of N-doped porous carbons were prepared by a facile one-pot KOH activating strategy from commercial urea formaldehyde resin (UF). The textural properties and nitrogen content of the N-doped carbons were carefully controlled by the activating temperature and KOH/UF mass ratios. As-prepared N-doped carbons show 3D block-shaped morphology, the BET surface area of up to 980 m2/g together with a pore volume of 0.52 cm3/g and N content of 23.51 wt%. The optimal adsorbent (UFK-600-0.2) presents a high CO2 uptake capacity of 4.03 mmol/g at 0 °C and 1 bar. Moreover, as-prepared N-doped carbon adsorbents show moderate isosteric heat of adsorption (43-53 kJ/mol), acceptable ideal adsorption solution theory (IAST) selectivity of 35 and outstanding recycling performance. It has been pointed out that while the CO2 uptake was mostly dependent on the textural feature, the N content of carbon also plays a critical role to define the CO2 adsorption performance. The present study delivers favorable N-doped carbon for CO2 uptake and provides a promising strategy for the design and synthesis of the carbon adsorbents.

| S-EPMC9610260 | biostudies-literature

Waste wool derived nitrogen-doped hierarchical porous carbon for selective CO2 capture.

Project description:The goal of this research is to develop a low-cost porous carbon adsorbent for selective CO2 capture. To obtain advanced adsorbents, it is critical to understand the synergetic effect of textural characteristics and surface functionality of the adsorbents for CO2 capture performance. Herein, we report a sustainable and scalable bio-inspired fabrication of nitrogen-doped hierarchical porous carbon by employing KOH chemical activation of waste wool. The optimal sample possesses a large surface area and a hierarchical porous structure, and exhibits good CO2 adsorption capacities of 2.78 mmol g-1 and 3.72 mmol g-1 at 25 °C and 0 °C, respectively, under 1 bar. Additionally, this sample also displays a moderate CO2/N2 selectivity, an appropriate CO2 isosteric heat of adsorption and a stable cyclic ability. These multiple advantages combined with the low-cost of the raw material demonstrate that this sample is an excellent candidate as an adsorbent for CO2 capture.

| S-EPMC9080743 | biostudies-literature

Integrated CO2 capture-fixation chemistry via interfacial ionic liquid catalyst in laminar gas/liquid flow.

Project description:Simultaneous capture of carbon dioxide (CO2) and its utilization with subsequent work-up would significantly enhance the competitiveness of CO2-based sustainable chemistry over petroleum-based chemistry. Here we report an interfacial catalytic reaction platform for an integrated autonomous process of simultaneously capturing/fixing CO2 in gas-liquid laminar flow with subsequently providing a work-up step. The continuous-flow microreactor has built-in silicon nanowires (SiNWs) with immobilized ionic liquid catalysts on tips of cone-shaped nanowire bundles. Because of the superamphiphobic SiNWs, a stable gas-liquid interface maintains between liquid flow of organoamines in upper part and gas flow of CO2 in bottom part of channel. The intimate and direct contact of the binary reagents leads to enhanced mass transfer and facilitating reactions. The autonomous integrated platform produces and isolates 2-oxazolidinones and quinazolines-2,4(1H,3H)-diones with 81-97% yields under mild conditions. The platform would enable direct CO2 utilization to produce high-valued specialty chemicals from flue gases without pre-separation and work-up steps.

| S-EPMC5343516 | biostudies-literature

Nitrogen-Rich Porous Organic Polymers with Supported Ag Nanoparticles for Efficient CO2 Conversion.

Project description:As CO2 emissions increase and the global climate deteriorates, converting CO2 into valuable chemicals has become a topic of wide concern. The development of multifunctional catalysts for efficient CO2 conversion remains a major challenge. Herein, two porous organic polymers (NPOPs) functionalized with covalent triazine and triazole N-heterocycles are synthesized through the copper(I)-catalyzed azide-alkyne cycloaddition (CuAAC) reaction. The NPOPs have an abundant microporous content and high specific surface area, which confer them excellent CO2 affinities with a CO2 adsorption capacity of 84.0 mg g-1 and 63.7 mg g-1, respectively, at 273 K and 0.1 MPa. After wet impregnation and in situ reductions, Ag nanoparticles were supported in the NPOPs to obtain Ag@NPOPs with high dispersion and small particle size. The Ag@NPOPs were applied to high-value conversion reactions of CO2 with propargylic amines and terminal alkynes under mild reaction conditions. The carboxylative cyclization transformation of propargylic amine into 2-oxazolidinone and the carboxylation transformation of terminal alkynes into phenylpropiolic acid had the highest TOF values of 1125.1 and 90.9 h-1, respectively. The Ag@NPOP-1 was recycled and used five times without any significant decrease in catalytic activity, showing excellent catalytic stability and durability.

| S-EPMC9501012 | biostudies-literature

Metal-Free Heptazine-Based Porous Polymeric Network as Highly Efficient Catalyst for CO2 Capture and Conversion.

Project description:The capture and catalytic conversion of CO2 into value-added chemicals is a promising and sustainable approach to tackle the global warming and energy crisis. The nitrogen-rich porous organic polymers are excellent materials for CO2 capture and separation. Herein, we present a nitrogen-rich heptazine-based microporous polymer for the cycloaddition reaction of CO2 with epoxides in the absence of metals and solvents. HMP-TAPA, being rich in the nitrogen site, showed a high CO2 uptake of 106.7 mg/g with an IAST selectivity of 30.79 toward CO2 over N2. Furthermore, HMP-TAPA showed high chemical and water stability without loss of any structural integrity. Besides CO2 sorption, the catalytic activity of HMP-TAPA was checked for the cycloaddition of CO2 and terminal epoxides, resulting in cyclic carbonate with high conversion (98%). They showed remarkable recyclability up to 5 cycles without loss of activity. Overall, this study represents a rare demonstration of the rational design of POPs (HMP-TAPA) for multiple applications.

| S-EPMC8554583 | biostudies-literature

Functional Porous Ionic Polymers as Efficient Heterogeneous Catalysts for the Chemical Fixation of CO2 under Mild Conditions.

Project description:The development of efficient and metal-free heterogeneous catalysts for the chemical fixation of CO2 into value-added products is still a challenge. Herein, we reported two kinds of polar group (-COOH, -OH)-functionalized porous ionic polymers (PIPs) that were constructed from the corresponding phosphonium salt monomers (v-PBC and v-PBH) using a solvothermal radical polymerization method. The resulting PIPs (POP-PBC and POP-PBH) can be used as efficient bifunctional heterogeneous catalysts in the cycloaddition reaction of CO2 with epoxides under relatively low temperature, ambient pressure, and metal-free conditions without any additives. It was found that the catalytic activities of the POP-PBC and POP-PBH were comparable with the homogeneous catalysts of Me-PBC and PBH and were higher than that of the POP-PPh3-COOH that was synthesized through a post-modification method, indicating the importance of the high concentration catalytic active sites in the heterogeneous catalysts. Reaction under low CO2 concentration conditions showed that the activity of the POP-PBC (with a conversion of 53.8% and a selectivity of 99.0%) was higher than that of the POP-PBH (with a conversion of 32.3% and a selectivity of 99.0%), verifying the promoting effect of the polar group (-COOH group) in the porous framework. The POP-PBC can also be recycled at least five times without a significant loss of catalytic activity, indicating the high stability and robustness of the PIPs-based heterogeneous catalysts.

| S-EPMC9269538 | biostudies-literature

Imine-Linked Polymer Based Nitrogen-Doped Porous Activated Carbon for Efficient and Selective CO2 Capture.

Project description:The preparation of nitrogen-doped activated carbon (NACs) has received significant attention because of their applications in CO2 capture and sequestration (CCS) owing to abundant nitrogen atoms on their surface and controllable pore structures by carefully controlled carbonization. We report high-surface-area porous N-doped activated carbons (NAC) by using soft-template-assisted self-assembly followed by thermal decomposition and KOH activation. The activation process was carried out under different temperature conditions (600-800 °C) using polyimine as precursor. The NAC-800 was found to have a high specific surface area (1900 m2 g-1), a desirable micropore size below 1 nm and, more importantly, a large micropore volume (0.98 cm3 g-1). NAC-800 also exhibits a significant capacity of CO2 capture i.e., over 6. 25 and 4.87 mmol g-1 at 273 K and 298 K respectively at 1.13 bar, which is one of among the highest values reported for porous carbons so far. Moreover, NAC also shows an excellent separation selectivity for CO2 over N2.

| S-EPMC5153834 | biostudies-literature

Construction of a BiVO4/VS-MoS2 S-scheme heterojunction for efficient photocatalytic nitrogen fixation.

Project description:Photocatalytic nitrogen (N2) reduction to ammonia (NH3), adopting H2O as the electron source, suffers from low efficiency owing to the sluggish kinetics of N2 reduction and the requirement of a substantial thermodynamic driving force. Herein, we present a straightforward approach for the construction of an S-scheme heterojunction of BiVO4/VS-MoS2 to successfully achieve photocatalytic N2 fixation, which is manufactured by coupling an N2-activation component (VS-MoS2 nanosheet) and water-oxidation module (BiVO4 nanocrystal) through electrostatic self-assembly. The VS-MoS2 nanosheet, enriched with sulfur vacancies, plays a pivotal role in facilitating N2 adsorption and activation. Additionally, the construction of the S-scheme heterojunction enhances the driving force for water oxidation and improves charge separation. Under simulated sunlight irradiation (100 mW cm-2), BiVO4/VS-MoS2 exhibits efficient photocatalytic N2 reduction activity with H2O as the proton source, yielding NH3 at a rate of 132.8 μmol g-1 h-1, nearly 7 times higher than that of pure VS-MoS2. This study serves as a noteworthy example of efficient N2 reduction to NH3 under mild conditions.

| S-EPMC10929607 | biostudies-literature

SO2 Capture Using Porous Organic Cages.

Project description:We report the first experimental investigation of porous organic cages (POCs) for the demanding challenge of SO2 capture. Three structurally related N-containing cage molecular materials were studied. An imine-functionalized POC (CC3) showed modest and reversible SO2 capture, while a secondary-amine POC (RCC3) exhibited high but irreversible SO2 capture. A tertiary amine POC (6FT-RCC3) demonstrated very high SO2 capture (13.78 mmol g-1 ; 16.4 SO2 molecules per cage) combined with excellent reversibility for at least 50 adsorption-desorption cycles. The adsorption behavior was investigated by FTIR spectroscopy, 13 C CP-MAS NMR experiments, and computational calculations.

| S-EPMC8361948 | biostudies-literature

Molten Salt Template Synthesis of Hierarchical Porous Nitrogen-Containing Activated Carbon Derived from Chitosan for CO2 Capture.

Project description:Here, hierarchical porous nitrogen-containing activated carbons (N-ACs) were prepared with LiCl-ZnCl2 molten salt as a template derived from cheap chitosan via simple one-step carbonization. The obtained N-ACs with the highest specific surface area of 2025 m2 g-1 and a high nitrogen content of 5.1 wt % were obtained using low molten salt/chitosan mass ratio (3/1) and moderate calcination temperature (1000 °C). Importantly, using these N-ACs as CO2 solid-state adsorbents, the maximum CO2 capture capacities could be up to 7.9/5.6 mmol g-1 at 0 °C/25 °C under 1 bar pressure, respectively. These CO2 capture capacities of N-ACs were the highest compared to reported biomass-derived carbon materials, and these values were also comparable to most of porous carbon materials. Moreover, as-made N-ACs also showed good selectivity for CO2/N2 separation and excellent recyclability. The unique hierarchical porous structure of N-ACs thus provided the right combination of adsorbent properties and could enable the design of high-performance CO2 solid adsorbents.

| S-EPMC7496027 | biostudies-literature