The engineering of highly organized systems from instructed molecular building blocks opens up new vistas for the control of matter and the exploration of nanodevice concepts. Recent investigations demonstrate that well-defined surfaces provide versatile platforms for steering and monitoring the assembly of molecular nanoarchitectures in exquisite detail. This review delineates the principles of noncovalent synthesis on metal substrates under ultrahigh vacuum conditions and briefly assesses the pertaining terminology-self-assembly, self-organization, and self-organized growth. It presents exemplary scanning-tunneling-microscopy observations, providing atomistic insight into the self-assembly of organic clusters, chains, and superlattices, and the metal-directed assembly of low-dimensional coordination architectures. This review also describes hierarchic-assembly protocols leading to intricate multilevel order. Molecular architectonic on metal surfaces represents a versatile rationale to realize structurally complex nanosystems with specific shape, composition, and functional properties, which bear promise for technological applications.

Molecular architectonic on metal surfaces.

More than 20 years ago, we published in Chemical Reviews a paper entitled “Intermolecular Interactions between Medium-Sized Systems. Nonempirical and Empirical Calculations of Interaction Energy: Successes and Failures”. The situation in calculations of noncovalent interactions at that time can be best characterized by the question we posed at the very beginning of the review: “Can quantum chemistry describe vdW (van der Waals; today we call it noncovalent) interactions as successfully as covalent interactions?” Our answer then was “unambiguously yes”. We had good reason for an optimistic “yes” since we presented the first coupledcluster calculations including triple excitations for a (at that time) large complexsthe water dimer. We stressed the importance of the triple excitations for noncovalent interactions, and in the section called Prospects, we wrote that “significant progress is highly desirable with beyond-SCF methods, where new, more accurate and efficient procedures are developed”. In this respect we were right, and in the past 20 years, we have witnessed an enormous growth of interest in the fast and accurate calculation of intermolecular interactions. What is the reason for such an interest, or more generally, why are noncovalent interactions so relevant in modern research? Is it the mere existence of noncovalent complexesmore » in the gas and liquid phases? Certainly not. The answer should be sought in the role that noncovalent interactions are playing in both bio- and nanostructures.« less

Stabilization and structure calculations for noncovalent interactions in extended molecular systems based on wave function and density functional theories.

Gold is an element whose unique properties are strongly influenced by relativistic effects. A large body of appropriate calculations now exists and its main conclusions are summarized in this critical review. The present paper completes the recent reviews by Pyykko (2004, 2005) (529 references).

Theoretical chemistry of gold. III

Textiles have been concomitant of human civilization for thousands of years. With the advances in chemistry and materials, integrating textiles with energy harvesters will provide a sustainable, environmentally friendly, pervasive, and wearable energy solution for distributed on-body electronics in the era of Internet of Things. This article comprehensively and thoughtfully reviews research activities regarding the utilization of smart textiles for harvesting energy from renewable energy sources on the human body and its surroundings. Specifically, we start with a brief introduction to contextualize the significance of smart textiles in light of the emerging energy crisis, environmental pollution, and public health. Next, we systematically review smart textiles according to their abilities to harvest biomechanical energy, body heat energy, biochemical energy, solar energy as well as hybrid forms of energy. Finally, we provide a critical analysis of smart textiles and insights into remaining challenges and future directions. With worldwide efforts, innovations in chemistry and materials elaborated in this review will push forward the frontiers of smart textiles, which will soon revolutionize our lives in the era of Internet of Things.

Smart Textiles for Electricity Generation.

The development of reliable anthropogenic emission inventories is essential for both understanding the sources of air pollution and designing effective air-pollution-control measures in China. However, it is challenging to quantify emissions in China accurately, given the variety of contributing sources, the complexity of the technology mix and the lack of reliable measurements. Over the last two decades, tremendous efforts have been made to improve the accuracy of emission inventories, and significant improvements have been realized. More reliable statistics and survey-based data have been used to reduce the uncertainties in activity rates and technology distributions. Local emission factors and source profiles covering various sources have been measured and reported. Based on these local databases, improved emission inventory models have been developed for power plants, large industrial plants and the residential, transportation and agricultural sectors. In this paper, we review the progress that has been made in developing inventories of anthropogenic emissions in China. We first highlight the major updates that have been made to emission inventory models and the underlying data by source category. We then summarize the sector-based estimates of emissions of different species contained in current inventories. The progress that has been made in the development of model-ready emissions is also presented. Finally, we suggest future directions for further improving the accuracy of emission inventories in China.

Anthropogenic emission inventories in China: a review

. A method is presented for the evaluation of the exhaust emissions of marine traffic, based on the messages provided by the Automatic Identification System (AIS), which enable the identification and location determination of ships. The use of the AIS data facilitates the positioning of ship emissions with a high spatial resolution, which is limited only by the inaccuracies of the Global Positioning System (typically a few metres) that is used in vessel navigation. The emissions are computed based on the relationship of the instantaneous speed to the design speed, and the detailed technical information of the engines of the ships. The modelling of emissions is also based on a few basic principles of ship design, including the modelling of the propelling power of each vessel in terms of its speed. We have investigated the effect of waves on the consumption of fuel, and on the emissions to the atmosphere. The predictions of fuel consumption were compared with the actual values obtained from the shipowners. For a Roll on – Roll off cargo/passenger ship (RoPax), the predicted and reported values of annual fuel consumption agreed within an accuracy of 6%. According to the data analysis and model computations, the emissions of NOx, SOx and CO2 originating from ships in the Baltic Sea during the full calendar year of 2007 were in total 400 kt, 138 kt and 19 Mt, respectively. A breakdown of emissions by flag state, the type of ship and the year of construction is also presented. The modelling system can be used as a decision support tool in the case of issues concerning, e.g., the health effects caused by shipping emissions or the construction of emission-based fairway dues systems or emissions trading. The computation of emissions can be automated, which will save resources in constructing emission inventories. Both the methodologies and the emission computation program can be applied in any sea region in the world, provided that the AIS data from that specific region are available.

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A modelling system for the exhaust emissions of marine traffic and its application in the Baltic Sea area

. A method is presented for the evaluation of the exhaust emissions of marine traffic, based on the messages provided by the Automatic Identification System (AIS), which enable the positioning of ship emissions with a high spatial resolution (typically a few tens of metres). The model also takes into account the detailed technical data of each individual vessel. The previously developed model was applicable for evaluating the emissions of NOx, SOx and CO2. This paper addresses a substantial extension of the modelling system, to allow also for the mass-based emissions of particulate matter (PM) and carbon monoxide (CO). The presented Ship Traffic Emissions Assessment Model (STEAM2) allows for the influences of accurate travel routes and ship speed, engine load, fuel sulphur content, multiengine setups, abatement methods and waves. We address in particular the modeling of the influence on the emissions of both engine load and the sulphur content of the fuel. The presented methodology can be used to evaluate the total PM emissions, and those of organic carbon, elemental carbon, ash and hydrated sulphate. We have evaluated the performance of the extended model against available experimental data on engine power, fuel consumption and the composition-resolved emissions of PM. We have also compared the annually averaged emission values with those of the corresponding EMEP inventory, As example results, the geographical distributions of the emissions of PM and CO are presented for the marine regions of the Baltic Sea surrounding the Danish Straits.

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Extension of an assessment model of ship traffic exhaust emissions for particulate matter and carbon monoxide

We evaluate public health and climate impacts of low-sulphur fuels in global shipping. Using high-resolution emissions inventories, integrated atmospheric models, and health risk functions, we assess ship-related PM2.5 pollution impacts in 2020 with and without the use of low-sulphur fuels. Cleaner marine fuels will reduce ship-related premature mortality and morbidity by 34 and 54%, respectively, representing a ~ 2.6% global reduction in PM2.5 cardiovascular and lung cancer deaths and a ~3.6% global reduction in childhood asthma. Despite these reductions, low-sulphur marine fuels will still account for ~250k deaths and ~6.4 M childhood asthma cases annually, and more stringent standards beyond 2020 may provide additional health benefits. Lower sulphur fuels also reduce radiative cooling from ship aerosols by ~80%, equating to a ~3% increase in current estimates of total anthropogenic forcing. Therefore, stronger international shipping policies may need to achieve climate and health targets by jointly reducing greenhouse gases and air pollution.

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Jukka-Pekka Jalkanen

Papers

A modelling system for the exhaust emissions of marine traffic and its application in the Baltic Sea area

Extension of an assessment model of ship traffic exhaust emissions for particulate matter and carbon monoxide

Cleaner fuels for ships provide public health benefits with climate tradeoffs

Global assessment of shipping emissions in 2015 on a high spatial and temporal resolution

Third IMO Greenhouse Gas Study 2014