Spontaneous Catalytic Paal–Knorr Reactions for N-Substituted Pyrrole Synthesis by Microdroplet Chemistry DOI
Jiayao Li, Jiannan Sun, Yizhou Wang

и другие.

ACS Sustainable Chemistry & Engineering, Год журнала: 2024, Номер 13(1), С. 571 - 582

Опубликована: Дек. 31, 2024

It is well recognized in recent studies that water molecules at the gas–liquid interface of microdroplets spontaneously dissociate into hydronium and hydroxide form superacids/superbases reactive species (hydrated electrons, radicals, hydrogen peroxide, radical cations/anions, etc.) due to 109 V m–1 electric field. In contrast extensive interest spontaneous redox reactions by microdroplet studies, limited attention has been attracted gram-scale organic synthesis catalyzed formed superacids/superbases. This study demonstrates catalysis superacids for Paal–Knorr reactions, one most classic pathways construct N-substituted pyrroles with biologically pharmaceutically important roles. can proceed no external catalysts isopropanol within 10 min room temperature. Sixteen were synthesized using method 83–99% yields, several orders magnitude reaction acceleration (a typical rate factor 1.18 × 103 based on ratio constants), a scale-up 5.50 g h–1. By avoiding catalysts, thermal irradiation, long times, problematic solvents required conventional methods, was green, efficient, attractive alternative construction their derivatives.

Язык: Английский

Atmospheric Hydroxyl Radical Route Revealed: Interface-Mediated Effects of Mineral-Bearing Microdroplet Aerosol DOI
Le Yang,

Yangyang Liu,

Qiuyue Ge

и другие.

Journal of the American Chemical Society, Год журнала: 2025, Номер unknown

Опубликована: Янв. 17, 2025

Hydroxyl radical (·OH) plays a crucial role in atmospheric chemistry, regulating the oxidative potential and aerosol composition. This study reveals an unprecedented source of ·OH atmosphere: mineral dust-bearing microdroplet aerosols. We demonstrate that Kaolin clay particles aerosols trigger rapid production upon solar irradiation, with rates reaching order at least 10-3 M s-1. rate is several orders magnitude higher than bulk phase (2.4 × 10-11 s-1) previously known pathways. On this basis, surface-based interfacial estimated to be 8.9 10-5 mol m-2 s-1 air-water-solid interface 1 μm sized particles. The enhanced formation attributed unique features interfaces, where lifespan photoinduced holes was significantly increased due presence strong electric fields air-water interface. further investigated impacts various environmental factors properties on production, including light intensity, relative humidity, particle size, pH. Our findings provide new insights into photochemical processes mediated by aerosols, which are important contributors atmosphere. work advances our understanding chemistry its profound lasting implications for air quality climate.

Язык: Английский

Процитировано

1
A comprehensive understanding on droplets DOI
Gang Chen, Guanhua Lin

Advances in Colloid and Interface Science, Год журнала: 2025, Номер unknown, С. 103490 - 103490

Опубликована: Март 1, 2025

Язык: Английский

Процитировано

1
Oxidation of Ammonia in Water Microdroplets Produces Nitrate and Molecular Hydrogen DOI
Xiaowei Song, Chanbasha Basheer, Yu Xia

и другие.

Environmental Science & Technology, Год журнала: 2024, Номер 58(36), С. 16196 - 16203

Опубликована: Авг. 23, 2024

Water microdroplets containing dissolved ammonia (30–300 μM) are sprayed through a copper oxide mesh with 200 μm average pore size, resulting in the formation of nitrate (NO3–) and release molecular hydrogen (H2). The products result from redox process that takes place at liquid–solid interface contact electrification, where no external potential is applied. Oxidation initiated by superoxide radical anions (O2–) originate oxygen air surrounding hydroxyl radicals (OH•) originating water–air interface. Two spin traps (TEMPO DMPO) capture these as well NH2OH+•, HNO, NO•, NO2•, NOOH, which detected mass spectrometry. We also directly observed N2O2–• same means. found atom molecule can be set free not only form H• but H2, using residue gas analyzer. oxidation significantly enhanced factor 3 when irradiated ultraviolet light (265 nm, 5 W). 35% 300 μM degraded within 20 μs, conversion rate estimated to 15 nmol·mg–1·h–1.

Язык: Английский

Процитировано

6
Scale-up of Microdroplet Reactors for Efficient CO2 Resource Utilization DOI

Xiemin Liu,

X LI,

Xinrong Wang

и другие.

Journal of the American Chemical Society, Год журнала: 2025, Номер unknown

Опубликована: Янв. 13, 2025

Two-phase reactions involving microdroplets have gained significant attention in recent years due to their unique ability catalyze and accelerate that typically do not occur under standard conditions by leveraging chemical physical effects at the micrometer-scale interface. In this work we innovatively developed a scaled-up microdroplet reactor for efficient resource utilization of CO2. The reaction liquid is sprayed form mist (d32 < 20 μm), facilitating complete contact with gaseous We explored spray properties parameters on continuous production organic carbonates from Remarkably, enhanced efficiency least 10-fold compared conventional high-pressure setups. Additionally, used computational fluid dynamics (CFD) simulations optimize process parameters, systematically studying scaling up device. Here, present insights into reactors CO2 conversion applications, supported robust data.

Язык: Английский

Процитировано

0
Enhanced sulfate formation in mixed biomass burning and sea-salt interactions mediated by photosensitization: effects of chloride, nitrogen-containing compounds, and atmospheric aging DOI Creative Commons
Rongzhi Tang,

Jialiang Ma,

Ruifeng Zhang

и другие.

Atmospheric chemistry and physics, Год журнала: 2025, Номер 25(1), С. 425 - 439

Опубликована: Янв. 13, 2025

Abstract. Discrepancies persist between modeled simulations and measured sulfate concentrations in the marine boundary layer, especially when air is influenced by biomass burning plumes. However, there has been a notable dearth of research conducted on interactions sea-salt aerosol plumes, impeding comprehensive understanding formation. This work studied formation mixing real (BB) extracts NaCl, mimicking internal mixtures BB particles. BB–NaCl particles had significantly higher rate than incense (IS)–NaCl For fresh particles, followed trend corn straw (CS)–NaCl > rice (RS)–NaCl wheat (WS)–NaCl IS–NaCl. The filter sample aging was achieved exposure to OH• generated from UV irradiation. After aging, RS–NaCl exhibited highest enhancement rates among all due RS NaCl. Bulk aqueous experiments spiked with NaCl using model photosensitizers (PSs) nitrogen-containing organic compounds (NOCs), pyrazine (CHN), 4-nitrocatechol (CHON) revealed positive effects chloride PS–CHON system negative PS–CHN Our suggests that reaching or near coastal areas can affect via photosensitizer-mediated reactions, potentially exacerbating pollution.

Язык: Английский

Процитировано

0
Carbonate radical ion as a key driver of rapid atmospheric sulfate formation DOI Creative Commons
Yangyang Liu, Wei Li,

Qiuyue Ge

и другие.

npj Climate and Atmospheric Science, Год журнала: 2025, Номер 8(1)

Опубликована: Фев. 12, 2025

Язык: Английский

Процитировано

0
Accelerated Pollutant Degradation by UV/H2O2 at the Air–Water Interface of Microdroplets DOI
Xiaochen Liu, Yishuai Pan, Yu Yao

и другие.

Environmental Science & Technology, Год журнала: 2025, Номер unknown

Опубликована: Март 6, 2025

Ultraviolet light-induced homolysis of hydrogen peroxide (UV/H2O2) can generate powerful hydroxyl radicals (•OH) for sustainable water purification. However, the efficiency conventional bulk-phase UV/H2O2 system is limited by low yield and utilization •OH, in turn necessitating high UV energy input long purification period. In this study, we present an innovative microdroplet enhanced pollutant degradation. The degradation pollutants sprayed microdroplets was accelerated 8.5-63.3-fold compared to those bulk water, demonstrating universal effectiveness across a range types diverse aqueous matrices. This enhancement stems from elevated •OH production at air-water interface due absorbance H2O2. 45-fold higher than that facilitating rapid •OH-mediated Moreover, accumulate interface, where concentrated, leading mediating before quenching. Our findings provide solution overcome bottlenecks utilization, offering insights improving treatment systems.

Язык: Английский

Процитировано

0
Dual-Function SERS Microdroplet Sensor for Rapid Differentiation of Influenza a and SARS-CoV-2 DOI

Xiangdong Yu,

Sohyun Park,

Younju Joung

и другие.

Analytical Chemistry, Год журнала: 2025, Номер unknown

Опубликована: Апрель 9, 2025

This study presents the development of a dual-function microdroplet sensor utilizing surface-enhanced Raman scattering (SERS) technology to identify and quantify Influenza A COVID-19 viruses. The proposed microfluidic device incorporates compartments for two-phase segmented droplet generation, merging, splitting, detection. Both viral strains were identified by isolating magnetic antibody-antigen complexes from liquid medium using magnetized bar embedded in channel. Concurrent spectroscopic readings obtained as suspended droplets containing residual SERS-active nanoparticles traversed interrogation zone focused laser beam. Precise quantitative analysis was accomplished correcting characteristic peak intensities both viruses with internal standards, while ensemble averaging signals multiple ensured high reproducibility. SERS represents novel vitro diagnostic approach capable rapidly distinguishing between sensitivity When coupled portable spectrophotometer, shows significant potential tool swift situ detection pathogens.

Язык: Английский

Процитировано

0
Air-water interface of microdroplet enhances photocatalytic oxidative species generation and utilization DOI

Kejian Li,

Wenbo You, Yucheng Zhu

и другие.

Journal of Hazardous Materials, Год журнала: 2025, Номер 493, С. 138311 - 138311

Опубликована: Апрель 25, 2025

Язык: Английский

Процитировано

0
Complexities of Photosensitization in Atmospheric Particles DOI Creative Commons
Zhancong Liang, Yongjie Li,

Brix Raphael Go

и другие.

ACS ES&T Air, Год журнала: 2024, Номер 1(11), С. 1333 - 1351

Опубликована: Окт. 10, 2024

Brown carbons (BrCs) play a pivotal role in the light absorption by aerosol particulates exerting positive radiative forcing effect that contributes to global warming. Beyond impacts on balance, some BrCs, as photosensitizers, can generate reactive triplet-state molecules toward various atmospheric upon photoexcitation. The significance of photosensitization has been increasingly recognized, particularly context escalated wildfire incidents emit substantial BrCs. We focus complex discussing current challenges, including (1) diverse reactivities photosensitizer mixture particles, (2) methodologies for investigating processes, (3) driving factors photosensitization, and (4) typical pathways mechanisms photosensitized reactions. Lastly, we advise future research refined parametrization triplet singlet oxygen concentrations, alongside their reactivities.

Язык: Английский

Процитировано

3