Dataset Information

Phosgene Synthesis Catalysis: The Influence of Small Quantities of Bromine in the Chlorine Feedstream.

ABSTRACT: The effect of relatively low concentrations of Br_2(g) in the Cl_2(g) feedstock for phosgene synthesis catalysis via the reaction of CO_(g) and Cl_2(g) over activated carbon (Donau Supersorbon K40) is explored. Under the stated reaction conditions and in the absence of a catalyst, BrCl_(g) forms from the reaction of Cl_2(g) and Br_2(g). Phosgene synthesis over the catalyst at 323 K is investigated for Br_2(g):Cl_2(g) molar flow ratios in the range 0-1.52% (0-15,190 ppm) and shows enhanced rates of phosgene production. Maximum phosgene production is observed at a Br_2(g):Cl_2(g) molar flow ratio of 1.52% (15,190 ppm), which corresponds to an enhancement in the rate of phosgene production of ∼227% with respect to the phosgene flow rate observed in the absence of an incident bromine co-feed. A reaction model is proposed to account for the experimental observables, where BrCl_(g) is highlighted as a significant intermediate. Specifically, enhanced rates of phosgene production are associated with the dissociative adsorption of BrCl_(g) that indirectly increases the pool of Cl_(ad) available for reaction.

SUBMITTER: Rossi GE

PROVIDER: S-EPMC8025734 | biostudies-literature | 2021 Mar

REPOSITORIES: biostudies-literature

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Phosgene Synthesis Catalysis: The Influence of Small Quantities of Bromine in the Chlorine Feedstream.

Rossi Giovanni E GE Winfield John M JM Meyer Nathalie N Jones Don H DH Carr Robert H RH Lennon David D

Industrial & engineering chemistry research 20210218 8

The effect of relatively low concentrations of Br2(g) in the Cl2(g) feedstock for phosgene synthesis catalysis via the reaction of CO(g) and Cl2(g) over activated carbon (Donau Supersorbon K40) is explored. Under the stated reaction conditions and in the absence of a catalyst, BrCl(g) forms from the reaction of Cl2(g) and Br2(g). Phosgene synthesis over the catalyst at 323 K is investigated for Br2(g):Cl ...[more]

PMID: 33840888

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Project description:As sources of reactive halogens, snowpacks in sea ice regions control the oxidative capacity of the Arctic atmosphere. However, measurements of snowpack halide concentrations remain sparse, particularly in the high Arctic, limiting our understanding of and ability to parameterize snowpack participation in tropospheric halogen chemistry. To address this gap, we measured concentrations of chloride, bromide, and sodium in snow samples collected during polar spring above remote multi-year sea ice (MYI) and first-year sea ice (FYI) north of Greenland and Alaska, as well as in the central Arctic, and compared these measurements to a larger dataset collected in the Alaskan coastal Arctic by Krnavek et al. (2012). Regardless of sea ice region, these surface snow samples generally featured lower salinities, compared to coastal snow. Surface snow in FYI regions was typically enriched in bromide and chloride compared to seawater, indicating snowpack deposition of bromine and chlorine-containing trace gases and an ability of the snowpack to participate further in bromine and chlorine activation processes. In contrast, surface snow in MYI regions was more often depleted in bromide, indicating it served as a source of bromine-containing trace gases to the atmosphere prior to sampling. Measurements at various snow depths indicate that the deposition of sea salt aerosols and halogen-containing trace gases to the snowpack surface played a larger role in determining surface snow halide concentrations compared to upward brine migration from sea ice. Calculated enrichment factors for bromide and chloride, relative to sodium, in the MYI snow samples suggests that MYI regions, in addition to FYI regions, have the potential to play an active role in Arctic boundary layer bromine and chlorine chemistry. The ability of MYI regions to participate in springtime atmospheric halogen chemistry should be considered in regional modeling of halogen activation and interpretation of satellite-based tropospheric bromine monoxide column measurements.

Dataset Information

Phosgene Synthesis Catalysis: The Influence of Small Quantities of Bromine in the Chlorine Feedstream.

Publications

Phosgene Synthesis Catalysis: The Influence of Small Quantities of Bromine in the Chlorine Feedstream.

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