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1. Sr _1-x Ca _x Fe _1-y Co _y O _3-δ as facile and tunable oxygen sorbents for chemical looping air separation

   https://doi.org/10.1088/2515-7655/ab7cb0  

   Dou, Jian ; Krzystowczyk, Emily ; Wang, Xijun ; Richard, Anthony R. ; Robbins, Thomas ; Li, Fanxing ( April 2020 , Journal of Physics: Energy)

   Chemical looping air separation (CLAS) is a promising technology for oxygen generation with high efficiency. The key challenge for CLAS is to design robust oxygen sorbents with suitable redox properties and fast redox kinetics. In this work, perovskite-structured Sr_1-xCa_xFe_1-yCo_yO₃oxygen sorbents were investigated and demonstrated for oxygen production with tunable redox properties, high redox rate, and excellent thermal/steam stability. Cobalt doping at B site was found to be highly effective, 33% improvement in oxygen productivity was observed at 500 °C. Moreover, it stabilizes the perovskite structure and prevents phase segregation under pressure swing conditions in the presence of steam. Scalable synthesis of Sr_0.8Ca_0.2Fe_0.4Co_0.6O₃oxygen sorbents was carried out through solid state reaction, co-precipitation, and sol-gel methods. Both co-precipitation and sol-gel methods are capable of producing Sr_0.8Ca_0.2Fe_0.4Co_0.6O₃sorbents with satisfactory phase purity, high oxygen capacity, and fast redox kinetics. Large scale evaluation of Sr_0.8Ca_0.2Fe_0.4Co_0.6O₃, using an automated CLAS testbed with over 300 g sorbent loading, further demonstrated the effectiveness of the oxygen sorbent to produce 95% pure O₂with a satisfactory productivity of 0.04 g_O2g_sorbent⁻¹h⁻¹at 600 °C.
2. A tailored multi-functional catalyst for ultra-efficient styrene production under a cyclic redox scheme

   https://doi.org/10.1038/s41467-021-21374-2  

   Zhu, Xing ; Gao, Yunfei ; Wang, Xijun ; Haribal, Vasudev ; Liu, Junchen ; Neal, Luke M. ; Bao, Zhenghong ; Wu, Zili ; Wang, Hua ; Li, Fanxing ( February 2021 , Nature Communications)

   Styrene is an important commodity chemical that is highly energy and CO₂intensive to produce. We report a redox oxidative dehydrogenation (redox-ODH) strategy to efficiently produce styrene. Facilitated by a multifunctional (Ca/Mn)_1−xO@KFeO₂core-shell redox catalyst which acts as (i) a heterogeneous catalyst, (ii) an oxygen separation agent, and (iii) a selective hydrogen combustion material, redox-ODH auto-thermally converts ethylbenzene to styrene with up to 97% single-pass conversion and >94% selectivity. This represents a 72% yield increase compared to commercial dehydrogenation on a relative basis, leading to 82% energy savings and 79% CO₂emission reduction. The redox catalyst is composed of a catalytically active KFeO₂shell and a (Ca/Mn)_1−xO core for reversible lattice oxygen storage and donation. The lattice oxygen donation from (Ca/Mn)_1−xO sacrificially stabilizes Fe³⁺in the shell to maintain high catalytic activity and coke resistance. From a practical standpoint, the redox catalyst exhibits excellent long-term performance under industrially compatible conditions.
3. Secondary organic aerosol formation from the β-pinene+NO₃ system: effect of humidity and peroxy radical fate

   https://doi.org/10.5194/acp-15-7497-2015  

   Boyd, C. M. ; Sanchez, J. ; Xu, L. ; Eugene, A. J. ; Nah, T. ; Tuet, W. Y. ; Guzman, M. I. ; Ng, N. L. ( January 2015 , Atmospheric Chemistry and Physics)

   Abstract. The formation of secondary organic aerosol (SOA) from the oxidation of β-pinene via nitrate radicals is investigated in the Georgia Tech Environmental Chamber (GTEC) facility. Aerosol yields are determined for experiments performed under both dry (relative humidity (RH) < 2 %) and humid (RH = 50 % and RH = 70 %) conditions. To probe the effects of peroxy radical (RO₂) fate on aerosol formation, "RO₂ + NO₃ dominant" and "RO₂ + HO₂ dominant" experiments are performed. Gas-phase organic nitrate species (with molecular weights of 215, 229, 231, and 245 amu, which likely correspond to molecular formulas of C₁₀H₁₇NO₄, C₁₀H₁₅NO₅, C₁₀H₁₇NO₅, and C₁₀H₁₅NO₆, respectively) are detected by chemical ionization mass spectrometry (CIMS) and their formation mechanisms are proposed. The NO⁺ (at m/z 30) and NO₂⁺ (at m/z 46) ions contribute about 11 % to the combined organics and nitrate signals in the typical aerosol mass spectrum, with the NO⁺ : NO₂⁺ ratio ranging from 4.8 to 10.2 in all experiments conducted. The SOA yields in the "RO₂ + NO₃ dominant" and "RO₂ + HO₂ dominant" experiments are comparable. For a wide range of organic mass loadings (5.1–216.1 μg m^&minus;3), the aerosol mass yield is calculated to be 27.0–104.1 %.more »Although humidity does not appear to affect SOA yields, there is evidence of particle-phase hydrolysis of organic nitrates, which are estimated to compose 45–74 % of the organic aerosol. The extent of organic nitrate hydrolysis is significantly lower than that observed in previous studies on photooxidation of volatile organic compounds in the presence of NO_x. It is estimated that about 90 and 10 % of the organic nitrates formed from the β-pinene+NO₃ reaction are primary organic nitrates and tertiary organic nitrates, respectively. While the primary organic nitrates do not appear to hydrolyze, the tertiary organic nitrates undergo hydrolysis with a lifetime of 3–4.5 h. Results from this laboratory chamber study provide the fundamental data to evaluate the contributions of monoterpene + NO₃ reaction to ambient organic aerosol measured in the southeastern United States, including the Southern Oxidant and Aerosol Study (SOAS) and the Southeastern Center for Air Pollution and Epidemiology (SCAPE) study.

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4. Lipid normalization and stable isotope discrimination in Pacific walrus tissues

   https://doi.org/10.1038/s41598-019-42095-z  

   Clark, Casey T. ; Horstmann, Lara ; Misarti, Nicole ( April 2019 , Scientific Reports)

   Analysis of stable carbon and nitrogen isotope values (δ¹³C and δ¹⁵N) of animal tissues can provide important information about diet, physiology, and movements. Interpretation of δ¹³C and δ¹⁵N values, however, is influenced by factors such as sample lipid content, tissue-specific isotope discrimination, and tissue turnover rates, which are typically species- and tissue-specific. In this study, we generated lipid normalization models for δ¹³C and investigated the effects of chemical lipid extractions on δ¹³C and δ¹⁵N in Pacific walrus (Odobenus rosmarus divergens) muscle, liver, and skin. We also evaluated tissue-specific isotope discrimination in walrus muscle, liver, skin, and bone collagen. Mean δ¹³C_lipid-freeof skin and bone collagen were similar, as were mean δ¹⁵N of muscle and liver. All other tissues differed significantly for both isotopes. Differences in δ¹³C_lipid-freeand δ¹⁵N among tissues agreed with published estimates of marine mammal tissue-specific isotope discrimination factors, with the exception of skin. The results of this work will allow researchers to gain a clearer understanding of walrus diet and the structure of Arctic food webs, while also making it possible to directly compare the results of contemporary walrus isotope research with those of historic and paleoecological studies.
5. Chemical characteristics of submicron particles at the central Tibetan Plateau: insights from aerosol mass spectrometry

   https://doi.org/10.5194/acp-18-427-2018  

   Xu, Jianzhong ; Zhang, Qi ; Shi, Jinsen ; Ge, Xinlei ; Xie, Conghui ; Wang, Junfeng ; Kang, Shichang ; Zhang, Ruixiong ; Wang, Yuhang ( January 2018 , Atmospheric Chemistry and Physics)

   Abstract. Recent studies have revealed a significant influx of anthropogenic aerosol from South Asia to the Himalayas and Tibetan Plateau (TP) during pre-monsoon period. In order to characterize the chemical composition, sources, and transport processes of aerosol in this area, we carried out a field study during June 2015 by deploying a suite of online instruments including an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-AMS) and a multi-angle absorption photometer (MAAP) at Nam Co station (90°57′E, 30°46′N; 4730ma.s.l.) at the central of the TP. The measurements were made at a period when the transition from pre-monsoon to monsoon occurred. The average ambient mass concentration of submicron particulate matter (PM₁) over the whole campaign was  ∼ 2.0µgm⁻³, with organics accounting for 68%, followed by sulfate (15%), black carbon (8%), ammonium (7%), and nitrate (2%). Relatively higher aerosol mass concentration episodes were observed during the pre-monsoon period, whereas persistently low aerosol concentrations were observed during the monsoon period. However, the chemical composition of aerosol during the higher aerosol concentration episodes in the pre-monsoon season was on a case-by-case basis, depending on the prevailing meteorological conditions and air mass transport routes. Mostmore »of the chemical species exhibited significant diurnal variations with higher values occurring during afternoon and lower values during early morning, whereas nitrate peaked during early morning in association with higher relative humidity and lower air temperature. Organic aerosol (OA), with an oxygen-to-carbon ratio (O∕C) of 0.94, was more oxidized during the pre-monsoon period than during monsoon (average O∕C ratio of 0.72), and an average O∕C was 0.88 over the entire campaign period, suggesting overall highly oxygenated aerosol in the central TP. Positive matrix factorization of the high-resolution mass spectra of OA identified two oxygenated organic aerosol (OOA) factors: a less oxidized OOA (LO-OOA) and a more oxidized OOA (MO-OOA). The MO-OOA dominated during the pre-monsoon period, whereas LO-OOA dominated during monsoon. The sensitivity of air mass transport during pre-monsoon with synoptic process was also evaluated with a 3-D chemical transport model.

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