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The U.S. Department of Energy’s Carbon Capture Simulation Initiative (CCSI) was initiated in 2010 to develop and deploy state-of-the-art computational modeling and simulation tools to accelerate the development of carbon capture technology.The first components of the CCSI Toolset have been deployed and demonstrated for the design and optimization of post-combustion solid sorbent capture systems. These computational tools provide new capabilities for integrating multi-scale modeling , optimization and uncertainty quantification to rapidly screen new concepts and , ultimately , enable smarter , more focused pilot and demonstration scale projects. The components include a set of detailed process models coupled with a process synthesis and design framework to facilitate development of complete , integrated carbon capture processes using advanced optimization techniques including deterministic superstructure-based methods and derivative-free optimization (DFO). This paper describes these components of the CCSI toolset and how they have been used to develop and optimize a capture process.