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Explaining global surface aerosol number concentrations in terms of primary emissions and particle formation

2010, Spracklen, D.V., Carslaw, K.S., Merikanto, J., Mann, G.W., Reddington, C.L., Pickering, S., Ogren, J.A., Andrews, E., Baltensperger, U., Weingartner, E., Boy, M., Kulmala, M., Laakso, L., Lihavainen, H., Kivekäs, N., Komppula, M., Mihalopoulos, N., Kouvarakis, G., Jennings, S.G., O'Dowd, C., Birmili, W., Wiedensohler, A., Weller, R., Gras, J., Laj, P., Sellegri, K., Bonn, B., Krejci, R., Laaksonen, A., Hamed, A., Minikin, A., Harrison, R.M., Talbot, R., Sun, J.

We synthesised observations of total particle number (CN) concentration from 36 sites around the world. We found that annual mean CN concentrations are typically 300–2000 cm−3 in the marine boundary layer and free troposphere (FT) and 1000–10 000 cm−3 in the continental boundary layer (BL). Many sites exhibit pronounced seasonality with summer time concentrations a factor of 2–10 greater than wintertime concentrations. We used these CN observations to evaluate primary and secondary sources of particle number in a global aerosol microphysics model. We found that emissions of primary particles can reasonably reproduce the spatial pattern of observed CN concentration (R2=0.46) but fail to explain the observed seasonal cycle (R2=0.1). The modeled CN concentration in the FT was biased low (normalised mean bias, NMB=−88%) unless a secondary source of particles was included, for example from binary homogeneous nucleation of sulfuric acid and water (NMB=−25%). Simulated CN concentrations in the continental BL were also biased low (NMB=−74%) unless the number emission of anthropogenic primary particles was increased or a mechanism that results in particle formation in the BL was included. We ran a number of simulations where we included an empirical BL nucleation mechanism either using the activation-type mechanism (nucleation rate, J, proportional to gas-phase sulfuric acid concentration to the power one) or kinetic-type mechanism (J proportional to sulfuric acid to the power two) with a range of nucleation coefficients. We found that the seasonal CN cycle observed at continental BL sites was better simulated by BL particle formation (R2=0.3) than by increasing the number emission from primary anthropogenic sources (R2=0.18). The nucleation constants that resulted in best overall match between model and observed CN concentrations were consistent with values derived in previous studies from detailed case studies at individual sites. In our model, kinetic and activation-type nucleation parameterizations gave similar agreement with observed monthly mean CN concentrations.

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Discovery of ZrCoBi based half Heuslers with high thermoelectric conversion efficiency

2018, Zhu, H., He, R., Mao, J., Zhu, Q., Li, C., Sun, J., Ren, W., Wang, Y., Liu, Z., Tang, Z., Sotnikov, A., Wang, Z., Broido, D., Singh, D.J., Chen, G., Nielsch, K., Ren, Z.

Thermoelectric materials are capable of converting waste heat into electricity. The dimensionless figure-of-merit (ZT), as the critical measure for the material's thermoelectric performance, plays a decisive role in the energy conversion efficiency. Half-Heusler materials, as one of the most promising candidates for thermoelectric power generation, have relatively low ZTs compared to other material systems. Here we report the discovery of p-type ZrCoBi-based half-Heuslers with a record-high ZT of ∼1.42 at 973 K and a high thermoelectric conversion efficiency of ∼9% at the temperature difference of ∼500 K. Such an outstanding thermoelectric performance originates from its unique band structure offering a high band degeneracy (N v) of 10 in conjunction with a low thermal conductivity benefiting from the low mean sound velocity (v m ∼2800 m s-1). Our work demonstrates that ZrCoBi-based half-Heuslers are promising candidates for high-temperature thermoelectric power generation.

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Carbon nanostructures as a multi-functional platform for sensing applications

2018, Mendes, R.G., Wróbel, P.S., Bachmatiuk, A., Sun, J., Gemming, T., Liu, Z., Rümmeli, M.H.

The various forms of carbon nanostructures are providing extraordinary new opportunities that can revolutionize the way gas sensors, electrochemical sensors and biosensors are engineered. The great potential of carbon nanostructures as a sensing platform is exciting due to their unique electrical and chemical properties, highly scalable, biocompatible and particularly interesting due to the almost infinite possibility of functionalization with a wide variety of inorganic nanostructured materials and biomolecules. This opens a whole new pallet of specificity into sensors that can be extremely sensitive, durable and that can be incorporated into the ongoing new generation of wearable technology. Within this context, carbon-based nanostructures are amongst the most promising structures to be incorporated in a multi-functional platform for sensing. The present review discusses the various 1D, 2D and 3D carbon nanostructure forms incorporated into different sensor types as well as the novel functionalization approaches that allow such multi-functionality.

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Variability of black carbon mass concentrations, sub-micrometer particle number concentrations and size distributions: results of the German Ultrafine Aerosol Network ranging from city street to High Alpine locations

2018, Sun, J., Birmili, W., Hermann, M., Tuch, T., Weinhold, K., Spindler, G., Schladitz, A., Bastian, S., Löschau, G., Cyrys, J., Gu, J., Flentje, H., Briel, B., Asbac, C., Kaminski, H., Ries, L., Sohme, R., Gerwig, H., Wirtz, K., Meinhardt, F., Schwerin, A., Bath, O., Ma, N., Wiedensohler, A.

This work reports the first statistical analysis of multi-annual data on tropospheric aerosols from the German Ultrafine Aerosol Network (GUAN). Compared to other networks worldwide, GUAN with 17 measurement locations has the most sites equipped with particle number size distribution (PNSD) and equivalent black carbon (eBC) instruments and the most site categories in Germany ranging from city street/roadside to High Alpine. As we know, the variations of eBC and particle number concentration (PNC) are influenced by several factors such as source, transformation, transport and deposition. The dominant controlling factor for different pollutant parameters might be varied, leading to the different spatio-temporal variations among the measured parameters. Currently, a study of spatio-temporal variations of PNSD and eBC considering the influences of both site categories and spatial scale is still missing. Based on the multi-site dataset of GUAN, the goal of this study is to investigate how pollutant parameters may interfere with spatial characteristics and site categories. © 2019 The Authors

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Discovery of TaFeSb-based half-Heuslers with high thermoelectric performance

2019, Zhu, H., Mao, J., Li, Y., Sun, J., Wang, Y., Zhu, Q., Li, G., Song, Q., Zhou, J., Fu, Y., He, R., Tong, T., Liu, Z., Ren, W., You, L., Wang, Z., Luo, J., Sotnikov, A., Bao, J., Nielsch, K., Chen, G., Singh, D.J., Ren, Z.

Discovery of thermoelectric materials has long been realized by the Edisonian trial and error approach. However, recent progress in theoretical calculations, including the ability to predict structures of unknown phases along with their thermodynamic stability and functional properties, has enabled the so-called inverse design approach. Compared to the traditional materials discovery, the inverse design approach has the potential to substantially reduce the experimental efforts needed to identify promising compounds with target functionalities. By adopting this approach, here we have discovered several unreported half-Heusler compounds. Among them, the p-type TaFeSb-based half-Heusler demonstrates a record high ZT of ~1.52 at 973 K. Additionally, an ultrahigh average ZT of ~0.93 between 300 and 973 K is achieved. Such an extraordinary thermoelectric performance is further verified by the heat-to-electricity conversion efficiency measurement and a high efficiency of ~11.4% is obtained. Our work demonstrates that the TaFeSb-based half-Heuslers are highly promising for thermoelectric power generation.

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Substrate Developments for the Chemical Vapor Deposition Synthesis of Graphene

2020, Shi, Q., Tokarska, K., Ta, H.Q., Yang, X., Liu, Y., Ullah, S., Liu, L., Trzebicka, B., Bachmatiuk, A., Sun, J., Fu, L., Liu, Z., Rümmeli, M.H.

Since the isolation of graphene and numerous demonstrations of its unique properties, the expectations for this material to be implemented in many future commercial applications have been enormous. However, to date, challenges still remain. One of the key challenges is the fabrication of graphene in a manner that satisfies processing requirements. While transfer of graphene can be used, this tends to damage or contaminate it, which degrades its performance. Hence, there is an important drive to grow graphene directly over a number of technologically important materials, viz., different substrate materials, so as to avoid the need for transfer. One of the more successful approaches to synthesis graphene is chemical vapor deposition (CVD), which is well established. Historically, transition metal substrates are used due to their catalytic properties. However, in recent years this has developed to include many nonmetal substrate systems. Moreover, both solid and molten substrate forms have also been demonstrated. In addition, the current trend to progress flexible devices has spurred interest in graphene growth directly over flexible materials surfaces. All these aspects are presented in this review which presents the developments in available substrates for graphene fabrication by CVD, with a focus primarily on large area graphene.