Bieber Paul, Darwish Ghinwa H, Algar W Russ, Borduas-Dedekind Nadine
Department of Chemistry, University of British Columbia, Vancouver, British Columbia V6T 1Z1, Canada.
J Chem Phys. 2024 Sep 7;161(9). doi: 10.1063/5.0213171.
Organic matter can initiate heterogeneous ice nucleation in supercooled water droplets, thereby influencing atmospheric cloud glaciation. Predicting the ice nucleation ability of organic matter-containing cloud droplets is challenging due to the unknown mechanism for templating ice. Here, we observed the presence of nanoparticles in aqueous samples of known ice-nucleating biopolymers cellulose and lignin, as well as in newly identified ice-nucleating biopolymers xylan and laminarin. Using our drop Freezing Ice Nuclei Counter (FINC), we measured the median ice nucleation temperature (T50) of xylan and of laminarin droplets of 2 μl to be -14.2 and -20.0 °C, respectively. Next, we characterized these samples using nanoparticle tracking analysis, and we detected and quantified nanoparticles with mean diameters between 132 and 267 nm. Xylan contained the largest nanoparticles and froze at higher temperatures. Xylan also dictated the freezing in a 1:1:1:1 mixture with cellulose, lignin, laminarin, and xylan. Filtration experiments down to 300 kDa with the xylan sample indicated that the presence of nanoparticles triggered freezing. Overall, only samples with mean diameters above 150 nm froze above -20 °C. Furthermore, we determined the ice-active site densities normalized to particle concentrations, surface area, and mass of the nanoparticles to show that the samples' nucleation site densities are similar to sea spray aerosols and nanometer-sized dust. The identification and characterization of xylan and laminarin as nanometer-sized ice-nucleating substances expands the growing list of organic matter capable of impacting cloud formation and thus climate.
有机物可在过冷水滴中引发异质冰核形成,从而影响大气云的冰川化。由于冰形成模板机制未知,预测含有机物的云滴的冰核形成能力具有挑战性。在这里,我们观察到在已知的冰核形成生物聚合物纤维素和木质素的水性样品中,以及在新鉴定的冰核形成生物聚合物木聚糖和海带多糖中存在纳米颗粒。使用我们的液滴冷冻冰核计数器(FINC),我们测量了2 μl木聚糖和海带多糖液滴的中位冰核形成温度(T50)分别为-14.2和-20.0°C。接下来,我们使用纳米颗粒跟踪分析对这些样品进行了表征,并检测和量化了平均直径在132至267 nm之间的纳米颗粒。木聚糖含有最大的纳米颗粒,并在较高温度下冻结。木聚糖还决定了与纤维素、木质素、海带多糖和木聚糖按1:1:1:1混合时的冻结情况。用木聚糖样品进行低至300 kDa的过滤实验表明,纳米颗粒的存在引发了冻结。总体而言,只有平均直径大于