Quantum Chemistry as a Tool for Addressing Global Energy Needs and Related Environmental Challenges

“能源”——化石燃料和核燃料的开采以及从这些和其他来源生产电力（或例如运输燃料）——是全球最大的单一产业。获得廉价而丰富的能源，“为地球提供动力”，是现代社会和生活方式的基础。由此产生的挑战也相应巨大，其中许多挑战与沿途产生的废物有关。事实上，由人类活动（主要是二氧化碳排放，燃烧化石燃料产生的废物）引起的全球变暖可能已经成为我们这个时代最紧迫的环境挑战。减少二氧化碳排放需要大规模发明、开发和部署碳中和能源生产。煤炭燃烧过程中释放出的汞（Hg）等化石燃料的其他废物也是有害的。同样，采矿、核能转换和武器生产造成的放射性污染是主要的环境挑战之一。在提议的研究中，我们将使用计算量子化学的工具来解决与整体能量主题相关的特定分子水平化学问题。具体来说，我们专注于(i)锕系化学，（ii）环境汞（Hg）化学，（iii）太阳能（无碳）能源，特别是染料敏化太阳能电池（DSSC）。迫切需要增加复杂性的新模型和方法，因此（iv）我们将开发新方法并使其他方法适应手头的问题。在区域(i)中，我们将集中于铀、镎和钚的环境化学，以及与“吃豆人”配体形成的配合物，该系统提供了对这些元素化学的基本见解。在区域（ii）中，我们将研究水系统和汞与冰的相互作用。对于DSSC研究，（iii），我们的目标是戏剧性的设备改进，通过计算研究新的DSSC染料。（iv）我们将开发新的溶剂化方法（溶液环境），并采用现代、高效和准确的方法，如高通量计算来解决手头的问题。

'Energy' - extraction of fossil and nuclear fuels and the production of electricity (or e.g. transportation fuels) from these and other sources - is the single largest global industry. Access to cheap and plentiful energy, 'powering the planet', underpins much of modern society and lifestyle. Resulting challenges are correspondingly huge, and many of these are related to the waste produced along the way. Indeed, global warming caused by human activity (primarily carbon dioxide emissions, the waste from burning fossil fuels) has emerged as perhaps the most pressing environmental challenge of our time. Reducing carbon dioxide emissions requires invention, development and deployment of carbon-neutral energy production on a large scale. Other waste products from fossil fuels such as mercury (Hg), liberated during coal combustion, are harmful as well. Likewise, radioactive contamination resulting from mining, nuclear energy conversion and weapons production is one of the leading environmental challenges. In the proposed research, we will use the tools of computational quantum chemistry to address specific molecular level chemical questions related to the overall energy theme. Specifically, we focus on (i) actinide chemistry, (ii) environmental mercury (Hg) chemistry, (iii) solar (carbon-free) energy, notably dye-sensitized solar cells (DSSC). An immediate need arises for new models and methods of increased complexity, and hence (iv) we will develop new methods and adapt others to the problems at hand. In area (i) we will concentrate on the environmental chemistry of uranium, neptunium and plutonium, as well as complexes formed with the 'pacman' ligand, a system that provides fundamental insight into the chemistry of these elements. In area (ii), we will study aqueous systems and the interaction of Hg with ice. For the DSSC research, (iii), we aim at dramatic device improvements, by computationally studying novel DSSC dyes. (iv) We will develop new methods for solvation (solution environment) and adapt modern, efficient and accurate methods such as high-throughput computing to the problems at hand.