Abstract. Delhi, India, routinely experiences some of the world's highest urban particulate matter concentrations. We established the Delhi Aerosol Supersite study to provide long-term characterization of the ambient submicron aerosol composition in Delhi. Here we report on 1.25 years of highly time-resolved speciated submicron particulate matter (PM1) data, including black carbon (BC) and nonrefractory PM1 (NR-PM1), which we combine to develop a composition-based estimate of PM1 (“C-PM1” = BC + NR-PM1) concentrations. We observed marked seasonal and diurnal variability in the concentration and composition of PM1 owing to the interactions of sources and atmospheric processes. Winter was the most polluted period of the year, with average C-PM1 mass concentrations of ∼210 µg m−3. The monsoon was hot and rainy, consequently making it the least polluted (C-PM1 ∼50 µg m−3) period. Organics constituted more than half of the C-PM1 for all seasons and times of day. While ammonium, chloride, and nitrate each were ∼10 % of the C-PM1 for the cooler months, BC and sulfate contributed ∼5 % each. For the warmer periods, the fractional contribution of BC and sulfate to C-PM1 increased, and the chloride contribution decreased to less than 2 %. The seasonal and diurnal variation in absolute mass loadings were generally consistent with changes in ventilation coefficients, with higher concentrations for periods with unfavorable meteorology – low planetary boundary layer height and low wind speeds. However, the variation in C-PM1 composition was influenced by temporally varying sources, photochemistry, and gas–particle partitioning. During cool periods when wind was from the northwest, episodic hourly averaged chloride concentrations reached 50–100 µg m−3, ranking among the highest chloride concentrations reported anywhere in the world. We estimated the contribution of primary emissions and secondary processes to Delhi's submicron aerosol. Secondary species contributed almost 50 %–70 % of Delhi's C-PM1 mass for the winter and spring months and up to 60 %–80 % for the warmer summer and monsoon months. For the cooler months that had the highest C-PM1 concentrations, the nighttime sources were skewed towards primary sources, while the daytime C-PM1 was dominated by secondary species. Overall, these findings point to the important effects of both primary emissions and more regional atmospheric chemistry on influencing the extreme particle concentrations that impact the Delhi megacity region. Future air quality strategies considering Delhi's situation in both a regional and local context will be more effective than policies targeting only local, primary air pollutants.
Well-defined palladium−gold nanoparticles (PdAuNPs) with randomly alloyed structures and broadly tunable compositions were studied in catalytic nitrite (NO 2 − ) reduction. The catalysts were synthesized using a microwave-assisted polyol coreduction method. Pd x Au 100−x NPs with systematically varied compositions (x = 18−83) were supported on amorphous silica (SiO 2 ) and studied as model catalysts for aqueous NO 2 − reduction in a batch reactor, using H 2 as the electron donor. The reactions followed pseudo-firstorder kinetics for ≥80% NO 2 − conversion. The Pd x Au 100−x NP-SiO 2 catalysts showed a volcano-like correlation between NO 2 − reduction activity and x; the highest activity was observed for Pd 53 Au 47 , with an associated first-order rate constant of 5.12 L min −1 g metal −1. Alloy NPs with greater proportions of Au were found to reduce the loss in catalytic activity due to sulfide fouling. Density functional theory calculations indicate that this is because Au weakens sulfur binding at PdAuNP surfaces due to atomic ensemble, electronic, and strain effects and thus reduces sulfur poisoning. The environmental relevance of the most active supported catalyst was evaluated by subjecting it to five cycles of catalytic NO 2 − reduction. The catalytic activity decreased over multiple cycles, but analysis of the postreaction Pd x Au 100−x NP-SiO 2 materials using complementary techniques indicated that there were no significant structural changes. Most importantly, we show that Pd x Au 100−x NP-SiO 2 alloys are significantly more active NO 2 − reduction catalysts in comparison to pure Pd catalysts.
Using archived social media data, the language signatures of people going through breakups were mapped. Text analyses were conducted on 1,027,541 posts from 6,803 Reddit users who had posted about their breakups. The posts include users’ Reddit history in the 2 y surrounding their breakups across the various domains of their life, not just posts pertaining to their relationship. Language markers of an impending breakup were evident 3 mo before the event, peaking on the week of the breakup and returning to baseline 6 mo later. Signs included an increase in I-words, we-words, and cognitive processing words (characteristic of depression, collective focus, and the meaning-making process, respectively) and drops in analytic thinking (indicating more personal and informal language). The patterns held even when people were posting to groups unrelated to breakups and other relationship topics. People who posted about their breakup for longer time periods were less well-adjusted a year after their breakup compared to short-term posters. The language patterns seen for breakups replicated for users going through divorce (n = 5,144; 1,109,867 posts) or other types of upheavals (n = 51,357; 11,081,882 posts). The cognitive underpinnings of emotional upheavals are discussed using language as a lens.
Abstract. The Indian national capital, Delhi, routinely experiences some of the world's highest urban particulate matter concentrations. While fine particulate matter (PM2.5) mass concentrations in Delhi are at least an order of magnitude higher than in many western cities, the particle number (PN) concentrations are not similarly elevated. Here we report on 1.25 years of highly time-resolved particle size distribution (PSD) data in the size range of 12–560 nm. We observed that the large number of accumulation mode particles – that constitute most of the PM2.5 mass – also contributed substantially to the PN concentrations. The ultrafine particle (UFP; Dp<100 nm) fraction of PNs was higher during the traffic rush hours and for daytimes of warmer seasons, which is consistent with traffic and nucleation events being major sources of urban UFPs. UFP concentrations were found to be relatively lower during periods with some of the highest mass concentrations. Calculations based on measured PSDs and coagulation theory suggest UFP concentrations are suppressed by a rapid coagulation sink during polluted periods when large concentrations of particles in the accumulation mode result in high surface area concentrations. A smaller accumulation mode for warmer months results in an increased UFP fraction, likely owing to a comparatively smaller coagulation sink. We also see evidence suggestive of nucleation which may also contribute to the increased UFP proportions during the warmer seasons. Even though coagulation does not affect mass concentrations, it can significantly govern PN levels with important health and policy implications. Implications of a strong accumulation mode coagulation sink for future air quality control efforts in Delhi are that a reduction in mass concentration, especially in winter, may not produce a proportional reduction in PN concentrations. Strategies that only target accumulation mode particles (which constitute much of the fine PM2.5 mass) may even lead to an increase in the UFP concentrations as the coagulation sink decreases.
<p><strong>Abstract.</strong> Delhi, India routinely experiences some of the world's highest urban particulate matter concentrations. We established the Delhi Aerosol Supersite campaign to provide long-term characterization of the ambient submicron aerosol composition in Delhi. Here we report on 1.25 years of highly time resolved speciated submicron particulate matter (PM1) data, including black carbon (BC) and non-refractory PM1 (NR-PM1), which we combine to develop a composition-based estimate of PM1 (&#8220;C-PM1&#8221; = BC + NR-PM1) concentrations.</p> <p> We observed marked seasonal and diurnal variability in the concentration and composition of PM1 owing to the interactions of sources and atmospheric processes. Winter was the most polluted period of the year with average C-PM1 mass concentrations of ~210 &#956;g m&#8722;3. Monsoon was hot and rainy, consequently making it the least polluted (C-PM1 ~50 &#956;g m&#8722;3) period. Organics constituted more than half of the C-PM1 for all seasons and times of day. While ammonium, chloride and nitrate each were ~10% of the C-PM1 for the cooler months, BC and sulfate contributed ~5% each. For the warmer periods, the fractional contribution of BC and sulfate to C-PM1 increased and the chloride contribution decreased to less than 2%. The seasonal and diurnal variation in absolute mass loadings were generally consistent with changes in ventilation coefficients, with higher concentrations for periods with unfavorable meteorology&#8212;low planetary boundary layer height and low wind speeds. However, the variation in C-PM1 composition was influenced by temporally varying sources, photochemistry and gas-particle partitioning. During cool periods when wind was from the northwest, episodic hourly averaged chloride concentrations reached 50&#8211;100 &#956;g m&#8722;3, ranking among the highest chloride concentrations reported anywhere in the world.</p> <p> We estimated the contribution of primary emissions and secondary processes to Delhi's submicron aerosol. Secondary species contributed almost 50&#8211;70% of Delhi's C-PM1 mass for the winter and spring months, and up to 60&#8211;80% for the warmer summer and monsoon months. For the cooler months that had the highest C-PM1 concentrations, the nighttime sources were skewed towards primary sources, while the daytime C-PM1 was dominated by secondary species. Overall, these findings point to the important effects of both primary emissions and more regional atmospheric chemistry on influencing the extreme particle concentrations that impact the Delhi megacity region. Future air quality strategies considering Delhi's situation in both a regional and local context will be more effective than policies targeting only local, primary air pollutants.</p>
The ongoing COVID-19 pandemic has raised concerns for many regarding personal and public health implications, financial security and economic stability. Alongside many other unprecedented challenges, there are increasing concerns over social isolation and mental health. We introduce Expressive Interviewingan interview-style conversational system that draws on ideas from motivational interviewing and expressive writing. Expressive Interviewing seeks to encourage users to express their thoughts and feelings through writing by asking them questions about how COVID-19 has impacted their lives. We present relevant aspects of the system's design and implementation as well as quantitative and qualitative analyses of user interactions with the system. In addition, we conduct a comparative evaluation with a general purpose dialogue system for mental health that shows our system's potential in helping users to cope with COVID-19 issues.
Most scientists agree that climate change is the largest existential threat of our time. Despite the magnitude of the threat, surprisingly few climate-related discussions take place on social media. What factors drive online discussions about climate change? In this study, we examined the occurrence of Reddit discussions around three types of climate-related events: natural disasters (e.g., hurricanes, wildfires), political events (i.e., 2016 United States Presidential election), and policy events (i.e., United States’ withdrawal from Paris Climate Agreement, release of IPCC report). The objective was to understand how different types of events influence collective action as measured by discussions of climate change. Six large US cities were selected based on the occurrence of at least one locally-relevant natural disaster since 2014. Posts (N = 4.4 million) from subreddits of the selected cities were collected to obtain a six-month period before and after local natural disasters as well as climate-related political and policy events (which applied equally to all cities). Climate change discussions increased significantly for all three types of events, with the highest discussion during the 2016 elections. Further, discussions returned to baseline levels within 2 months following natural disasters and policy events but continued at elevated rates for up to 4 months following the 2016 elections. The findings suggest that collective discussions on climate change are driven more by political leaders’ controversial positions than life-threatening local natural disasters themselves. Implications for collective action are discussed.
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