Zinc-air batteries have recently attracted considerable interest owing to the larger storage capacity and lower cost compared to their lithium-ion counterparts. Electrode catalysts for the oxygen ...reduction reaction (ORR) and oxygen evolution reaction (OER) play a critical role in the operation of rechargeable zinc-air batteries. Herein, we report a simple and scalable strategy to fabricate porous carbon polyhedra using Zn-doped Co-based zeolitic imidazolate frameworks (ZnCo-ZIFs) as precursors. Strikingly, Zn doping leads to smaller Co nanoparticles and higher nitrogen content, which in turn enhances the ORR and OER activities of the obtained porous carbon polyhedra. The synergistic effect of the N-doped carbon and cobalt nanoparticles in the composite, the improved conductivity resulting from the high graphitization of carbon, and the large surface area of the porous polyhedral structure resulted in porous carbon polyhedra with excellent ORR and OER electrocatalytic activity in alkaline media. More importantly, air cathodes based on the optimal porous carbon polyhedra further exhibited superior performance to Pt/C catalysts in primary and rechargeable zinc-air batteries.
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EMUNI, FIS, FZAB, GEOZS, GIS, IJS, IMTLJ, KILJ, KISLJ, MFDPS, NLZOH, NUK, OBVAL, OILJ, PNG, SAZU, SBCE, SBJE, SBMB, SBNM, UKNU, UL, UM, UPUK, VKSCE, ZAGLJ
A growing body of literature discusses the CO2 emissions of cities. Still, little is known about black carbon (BC), a short-lived warming agent. Identifying the drivers of urban BC emissions is ...crucial for targeting cleanup efforts. A consumption-based approach enables all emissions to be allocated along the production chain to the product and place of final consumption, whereas a production approach attributes emissions to the place where goods and services are produced. In this study, we calculate the production-based and consumption-based emissions in 2012 in four Chinese megacities: Beijing, Shanghai, Tianjin and Chongqing. The results show that capital formation is the largest contributor, accounting for 37%–69% of consumption-based emissions. Approximately 44% of BC emissions related to goods consumed in Chongqing and more than 60% for Beijing, Shanghai and Tianjin occur outside of the city boundary. The large gap between consumption and production-based emissions can be attributed to the great difference in embodied emission intensities. Therefore, collaborative efforts to reduce emission intensity can be effective in mitigating climate change for megacities as either producers or consumers.
•We calculate consumption-based black carbon emissions for four Chinese megacities.•Capital formation is the largest contributor to consumption-based emissions.•44%–66% of consumption-based emissions are embodied in imports.•Large net imported emissions are attributable to a relatively lower emission intensity.
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GEOZS, IJS, IMTLJ, KILJ, KISLJ, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UL, UM, UPCLJ, UPUK, ZRSKP
Transition metal phosphides have great potential to optimize a number of functionalities in several energy conversion and storage applications, particularly when nanostructured or in nanoparticle ...form. However, the synthesis of transition metal phosphide nanoparticles and its scalability is often limited by the toxicity, air sensitivity, and high cost of the reagents used. We present here a simple, scalable, and cost-effective “heating up” procedure to produce metal phosphides using inexpensive, low-toxicity, and air-stable triphenyl phosphite as source of phosphorus and chlorides as metal precursors. This procedure allows the synthesis of a variety of phosphide nanoparticles, including phosphides of Ni, Co, and Cu. The use of carbonyl metal precursors further allowed the synthesis of Fe2P and MoP nanoparticles. The fact that minor modifications in the experimental parameters allowed producing nanoparticles with different compositions and even to tune their size and shape shows the high potential and versatility of the triphenyl phosphite precursor and the presented method. We also detail here a methodology to displace organic ligands from the surface of phosphide nanoparticles, which is a key step toward their application in energy conversion and storage systems.
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IJS, KILJ, NUK, PNG, UL, UM
•We developed a three-scale energy-related PM emissions intensity database.•Half of the direct energy-related PM emissions in Beijing were associated with exports.•Beijing outsourced approximately ...80% of its demand-driven PM emissions.•Beijing was a net exporter of PM emissions in domestic trade by importing metal, construction and chemical products.•Beijing was a net importer of PM emissions in international trade by exporting construction and leasing.
Particulate matter (PM) adversely affects air quality, human health and the climate, and it is more prevalent in urban areas. Few efforts have been made to quantify the impact of trade on PM concentrations in an urban economy. This paper presents an analysis of the impacts of domestic and international trade on PM emissions in Beijing using a three-scale input–output model, supported by the national and global embodied energy-related PM2.5, PM10 and TSP (total suspended particulate) emission intensities. The results found that the total energy-related PM2.5, PM10 and TSP emissions (production-based) in Beijing were 106Gg, 163Gg and 347Gg, respectively, in 2010. Of these amounts, 48% (51Gg, 74Gg and 146Gg, respectively) was associated with local demand, 42% (44Gg, 73Gg and 168Gg, respectively) was associated with domestic exports, and 10% (11Gg, 16Gg and 33Gg, respectively) was associated with international exports. From a consumption perspective, Beijing’s PM2.5, PM10 and TSP emissions were more than double the production-based PM emissions. Approximately 75% (172Gg, 311Gg and 786Gg, respectively) of the consumption-based PM emissions were domestically outsourced to other provinces, primarily via the import of metal (32Gg, 58Gg and 151Gg), construction (26Gg, 36Gg and 91Gg) and chemical products (16Gg, 30Gg and 75Gg), and 3% (8Gg, 10Gg and 24Gg, respectively) of consumption-based PM emissions were outsourced abroad. Our results indicate that domestic trade plays a dominant role in Beijing’s PM2.5 emissions. These findings suggest that more national and sub-national government should co-ordinate design and implement effective mechanisms to alleviate urban air pollution because of the significant effects of interprovincial and international trade on local emissions.
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GEOZS, IJS, IMTLJ, KILJ, KISLJ, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UL, UM, UPCLJ, UPUK, ZRSKP
Pulsed lasers operating in the mid-infrared (3-20 μm) are important for a wide range of applications in sensing, spectroscopy, imaging and communications. Despite recent advances with mid-infrared ...gain platforms, the lack of a capable pulse generation mechanism remains a significant technological challenge. Here we show that bulk Dirac fermions in molecular beam epitaxy grown crystalline Cd
As
, a three-dimensional topological Dirac semimetal, constitutes an exceptional ultrafast optical switching mechanism for the mid-infrared. Significantly, we show robust and effective tuning of the scattering channels of Dirac fermions via an element doping approach, where photocarrier relaxation times are found flexibly controlled over an order of magnitude (from 8 ps to 800 fs at 4.5 μm). Our findings reveal the strong impact of Cr doping on ultrafast optical properties in Cd
As
and open up the long sought parameter space crucial for the development of compact and high-performance mid-infrared ultrafast sources.
With the advantages of large field of view, low cost and simple structure, the freeform optical system has extensive requirements in space exploration and other fields. However, the current machining ...methods for freeform are difficult to meet the requirements of optical use. Based on a developed fast servo tool (FTS) device, this paper proposes an error compensation turning method for freeforms. Firstly, the Zernike polynomial fitting method is used to reconstruct the freeform surface shape error obtained from off-line measurement, and the offset compensation is used to correct the tool path. Then, the compensation processing physical system is built to simulate the off-line compensation processing of the workpiece to verify the feasibility of compensation processing. Finally, the turning compensation processing of convex freeform aluminum mirror is carried out, and the surface accuracy of the workpiece meets the requirements of visible band. The research results have important practical significance for realizing the fast response machining of free-form surface mirror.
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DOBA, IZUM, KILJ, NUK, PILJ, PNG, SAZU, SIK, UILJ, UKNU, UL, UM, UPUK
Inferring the demographic history of a population is essential in population genetic studies. Though the inference methods based on the sequentially Markov coalescent can present the population ...history in detail, these methods assume that the population size remains unchanged in each time interval during discretizing the hidden state in the hidden Markov model. Therefore, these methods fail to uncover the detailed population history in each time interval.
We present a new method called Beta-PSMC, which introduces the probability density function of a beta distribution with a broad variety of shapes into the Pairwise Sequentially Markovian Coalescent (PSMC) model to refine the population history in each discretized time interval in place of the assumption that the population size is unchanged. Using simulation, we demonstrate that Beta-PSMC can uncover more detailed population history, and improve the accuracy and resolution of the recent population history inference. We also apply Beta-PSMC to infer the population history of Adélie penguin and find that the fluctuation in population size is contrary to the temperature change 15-27 thousand years ago.
Beta-PSMC extends PSMC by allowing more detailed fluctuation of population size in each discretized time interval with the probability density function of beta distribution and will serve as a useful tool for population genetics.
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DOBA, IZUM, KILJ, NUK, PILJ, PNG, SAZU, SIK, UILJ, UKNU, UL, UM, UPUK
In this paper, switched Z-source/quasi-Z-source dc-dc converters (SZSC/SQZSCs) are proposed for the photovoltaic (PV) grid-connected power system, where the high step-up dc-dc converters are required ...to boost the low voltage to high voltage. The boost factor is increased by adding another one switch and diode to the output terminals of traditional Z-source/quasi-Z-source dc-dc converters. Not only does the output capacitor function as the filter capacitor; it is also connected in series into the inductors' charging loops when both switches are turned on. Compared with existing Z-source based structures, higher boost factor is realized through a small duty cycle (smaller than 0.25). On the one hand, the instability caused by the saturation of the inductors can be avoided. On the other hand, a larger range can be reserved for the modulation index of the backend H-bridge when they are used for the dc-ac conversion. Moreover, much fewer passive components are employed when compared with the recently proposed hybrid 3-Z-network topologies that have the same voltage gain, which can enhance the power density and decrease the cost. The performances of the proposed converters, including their operational principles in continuous and discontinuous current modes, voltage and current parameters of components, and impacts of parasitic parameters, are analyzed. The simulation and experimental results are given to verify the aforementioned characteristics and theoretical analysis.
Emission quantification of primary particulate matter (PM) is essential for assessment of its related climate and health impacts. To reduce uncertainty associated with global emissions of PM2.5, ...PM10, and TSP, we compiled data with high spatial (0.1° × 0.1°) and sectorial (77 primary sources) resolutions for 2007 based on a newly released global fuel data product (PKU-FUEL-2007) and an emission factor database. Our estimates for developing countries are higher than those previously reported. Spatial bias associated with large countries could be reduced by using subnational fuel consumption data. Additionally, we looked at temporal trends from 1960 to 2009 at country-scale resolution. Although total emissions are still increasing in developing countries, their intensities in terms of gross domestic production or energy consumption have decreased. PM emitted in developed countries is finer owing to a larger contribution from nonindustrial sources and use of abatement technologies. In contrast, countries like China, with strong industry emissions and limited abatement facilities, emit coarser PM. The health impacts of PM are intensified in hotspots and cities owing to covariance of sources and receptors. Although urbanization reduces the per person emission, overall health impacts related to these emissions are heightened because of aggregation effects.
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IJS, KILJ, NUK, PNG, UL, UM
Single-atom catalysts (SACs) show great promise in various applications due to their maximal atom utilization efficiency. However, the controlled synthesis of SACs with appropriate porous structures ...remains a challenge that must be overcome to address the diffusion issues in catalysis. Resolving these diffusion issues has become increasingly important because the intrinsic activity of the catalysts is dramatically improved by spatially isolated single-atom sites. Herein, we develop a facile topo-conversion strategy for fabricating hollow mesoporous metal-nitrogen-carbon SACs with enhanced diffusion for catalysis. Several hollow mesoporous metal-nitrogen-carbon SACs, including Co, Ni, Mn and Cu, are successfully fabricated by this strategy. Taking hollow mesoporous cobalt-nitrogen-carbon SACs as a proof-of-concept, diffusion and kinetic experiments demonstrate the enhanced diffusion of hollow mesoporous structures compared to the solid ones, which alleviates the bottleneck of poor mass transport in catalysis, especially involving larger molecules. Impressively, the combination of superior intrinsic activity from Co-N
sites and the enhanced diffusion from the hollow mesoporous nanoarchitecture significantly improves the catalytic performance of the oxidative coupling of aniline and its derivatives.