MOF Materials for the Capture of Highly Toxic H₂S and SO₂

Organometallics, Journal Year: 2020, Volume and Issue: 39(7), P. 883 - 915

Published: Jan. 15, 2020

Metal–organic frameworks (MOFs) are some of the most interesting and promising candidates to sequester toxic H2S SO2 gases. MOFs show advantages over classic porous materials due their chemical composition, ligand functionality, cavity dimensions, ease preparation, relatively low cost reactivation. The optimization physical–chemical interactions between molecules is key further amplification capture. Reversibility after adsorption can be modulated through noncovalent bonding functionalized ligands (within MOF structures) SO2. This review aims summarize recent advances in development MOF-based systems for capture removal We anticipate that this article offer very useful information on significant rapid progress enhancement by MOFs.

Language: Английский

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Understanding the deposition and reaction mechanism of ammonium bisulfate on a vanadia SCR catalyst: A combined DFT and experimental study

Applied Catalysis B Environment and Energy, Journal Year: 2019, Volume and Issue: 260, P. 118168 - 118168

Published: Sept. 6, 2019

Language: Английский

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A Colorimetric Artificial Olfactory System for Airborne Improvised Explosive Identification

Advanced Materials, Journal Year: 2020, Volume and Issue: 32(14)

Published: Jan. 29, 2020

Abstract The detection of ultralow or nonvolatile target analytes remains a significant challenge for artificial olfactory systems even after decades development, which severely limits their widespread application. To overcome this challenge, an system based on colorimetric hydrogel array is constructed the first time as universal representative. As effective extension conventional that integrates merits its predecessors, proposed accurately mimics mucosa and specific odorant binding proteins using hydrogels endowed with reagents hypochlorite, chlorate, perchlorate, urea, nitrate. Therefore, capable detecting discriminating between these five airborne improvised explosive microparticulates limit low 39.4 pg. Additionally, demonstrates good reusability over ten cycles, rapid response ≈0.2 s, excellent discrimination properties, despite variation. This proof‐of‐concept study yields novel strategy direct discriminative microparticulates.

Language: Английский

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Atmospheric Sulfuric Acid‐Dimethylamine Nucleation Enhanced by Trifluoroacetic Acid

Geophysical Research Letters, Journal Year: 2020, Volume and Issue: 47(2)

Published: Jan. 8, 2020

Abstract Sulfuric acid (SA)‐dimethylamine (DMA)‐H 2 O cluster formation has been proven to be responsible for a significant part of new particle (NPF) in Chinese megacity. However, the possible involvement common atmospheric acids subsequent growth SA‐DMA clusters remains elusive. We simulated and using relevant concentrations SA, DMA, trifluoroacetic (TFA), commonly observed perfluorocarboxylic acid, Density Functional Theory combined with Atmospheric Cluster Dynamics Code. The presence TFA leads complex routes an enhancement NPF rates by up 2.3 ([TFA] = 5.0 × 10 6 molecules cm −3 , [SA] 1.0 [DMA] 1.5 9 ). agreement (SA) 1 ·(DMA) 1‐2 ·(TFA) between simulations ambient measurements during events validates model predictions implies that could potentially boost rates.

Language: Английский

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Engineering surface framework TiO6 single sites for unprecedented deep oxidative desulfurization

National Science Review, Journal Year: 2024, Volume and Issue: 11(5)

Published: March 6, 2024

ABSTRACT Catalytic oxidative desulfurization (ODS) using titanium silicate catalysts has emerged as an efficient technique for the complete removal of organosulfur compounds from automotive fuels. However, precise control highly accessible and stable-framework Ti active sites remains challenging. Here we reveal first time by density functional theory calculations that framework hexa-coordinated (TiO6) species mesoporous silicates are most ODS lead to a lower-energy pathway ODS. A novel method achieve homogeneously distributed TiO6 single at surface been developed. Such exhibit exceptional performance. 920 ppm benzothiophene is achieved 60°C in 60 min, which 1.67 times best catalyst reported so far. For bulky molecules such 4,6-dimethyldibenzothiophene (DMDBT), it takes only 3 min remove 500 DMDBT with our catalyst, five faster than current catalyst. can be easily upscaled could used concrete industrial application minimized energy consumption high reaction efficiency.

Language: Английский

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Mechanistic insight into the competition between interfacial and bulk reactions in microdroplets through N2O5 ammonolysis and hydrolysis

Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)

Published: March 15, 2024

Abstract Reactive uptake of dinitrogen pentaoxide (N 2 O 5 ) into aqueous aerosols is a major loss channel for NO x in the troposphere; however, quantitative understanding mechanism lacking. Herein, computational chemistry strategy developed employing high-level quantum chemical methods; method offers detailed molecular insight hydrolysis and ammonolysis mechanisms N microdroplets. Specifically, our calculations estimate bulk interfacial rates to be (2.3 ± 1.6) × 10 −3 (6.3 4.2) −7 ns −1 , respectively, competes with at NH 3 concentrations above 1.9 −4 mol L . The slow rate suggests that processes have negligible effect on liquid water. In contrast, water dominated by due high rate. Our findings are applicable high-chemical complexity

Language: Английский

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Piperazine Enhancing Sulfuric Acid-Based New Particle Formation: Implications for the Atmospheric Fate of Piperazine

Environmental Science & Technology, Journal Year: 2019, Volume and Issue: 53(15), P. 8785 - 8795

Published: June 25, 2019

Piperazine (PZ), a cyclic diamine, is one of 160 detected atmospheric amines and an alternative solvent to the widely used monoethanolamine in post-combustion CO2 capture. Participating H2SO4 (sulfuric acid, SA)-based new particle formation (NPF) could be important removal pathway for PZ. Here, we employed quantum chemical calculations kinetics modeling evaluate enhancing potential PZ on SA-based NPF by examining PZ-SA clusters. The results indicate that behaves more like monoamine stabilizing SA can enhance at parts per trillion (ppt) level. less than chainlike diamine putrescine greater dimethylamine, which strongest agents confirmed ambient observations experiments. After initial (PZ)1(SA)1 cluster, cluster mainly grows gradual addition or monomer, followed cluster. We find ratio combination oxidations 0.5-0.97 278.15 K. As result, conclude participation significantly alter environmental impact compared only considering oxidation pathways.

Language: Английский

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Unprecedented Ambient Sulfur Trioxide (SO₃) Detection: Possible Formation Mechanism and Atmospheric Implications

Environmental Science & Technology Letters, Journal Year: 2020, Volume and Issue: 7(11), P. 809 - 818

Published: Sept. 25, 2020

Sulfur trioxide (SO3) is a crucial compound for atmospheric sulfuric acid (H2SO4) formation, rain and other physicochemical processes. During the daytime, SO3 mainly produced from photo-oxidation of SO2 by OH radicals. However, sources during early morning night, when radicals are scarce, not fully understood. We report results two field measurements in urban Beijing winter summer 2019, using nitrate-CI-APi-LTOF (chemical ionization-atmospheric pressure interface-long-time-of-flight) mass spectrometer to detect H2SO4. Our show level was higher than summer, with high levels observed especially (∼05:00 ∼08:30) night (∼18:00 ∼05:00 next day). On basis analysis SO2, NO x , black carbon, traffic flow, ions, we suggest could be formed catalytic oxidation on surface traffic-related carbon. This previously unidentified source significant H2SO4 formation thus promotes sub-2.5 nm particle formation. These findings will help understanding formulating policies mitigate secondary Chinese megacities.

Language: Английский

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NWPEsSe: An Adaptive-Learning Global Optimization Algorithm for Nanosized Cluster Systems

Journal of Chemical Theory and Computation, Journal Year: 2020, Volume and Issue: 16(6), P. 3947 - 3958

Published: May 4, 2020

Global optimization constitutes an important and fundamental problem in theoretical studies many chemical fields, such as catalysis, materials, or separations problems. In this paper, a novel algorithm has been developed for the global of large systems including neat ligated clusters gas phase supported periodic boundary conditions. The method is based on updated artificial bee colony (ABC) method, that allows adaptive-learning during search process. new tested against four classes diverse nature: Au55, Au82+, Au8 graphene oxide defected rutile, cluster assembly [Co6Te8(PEt3)6][C60]n, with sizes ranging between 1 3 nm containing up to 1300 atoms. Reliable minima (GMs) are obtained all cases, either confirming published data reporting lower energy structures. interface other codes form independent program, Northwest Potential Energy Search Engine (NWPEsSe), freely available, it provides powerful efficient approach nanosized systems.

Language: Английский

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Global optimization of chemical cluster structures: Methods, applications, and challenges

International Journal of Quantum Chemistry, Journal Year: 2020, Volume and Issue: 121(7)

Published: Nov. 21, 2020

Abstract Chemical clusters are relevant to many applications in catalysis, separations, materials, and energy sciences. Experimentally, the structure of is difficult determine, but it very important understanding their chemistry properties. Computational methods can be used examine cluster structure, however finding most stable not simple, particularly as size increases. Global optimization techniques have long been tackle problem such approaches would look for a global minimum, while sampling local minima over whole potential surface well. In this review, state‐of‐the‐art theory summarized. First, definition, significance, relation experiments, brief history presented. We then discuss, more detail, three versatile methods: basin hopping, artificial bee colony algorithm, genetic algorithm. close with some representative application examples since 2016 challenges, open questions opportunities field.

Language: Английский

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