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There is growing interest in using hydrogen (H2) as a long-duration energy storage resource in a future electric grid dominated by variable renewable energy (VRE) generation. Modeling H2 use exclusively for grid-scale energy storage, often referred to as “power-to-gas-to-power (P2G2P)”, overlooks the cost-sharing and CO2 emission benefits from using the deployed H2 assets to decarbonize other end-use sectors where direct electrification is challenging. Here, we develop a generalized framework for co-optimizing infrastructure investments across the electricity and H2 supply chains, accounting for the spatio-temporal variations in energy demand and supply. We apply this sector-coupling framework to the U.S. Northeast under a range of technology cost and carbon price scenarios and find greater value of power-to-H2 (P2G) vs. P2G2P routes. Specifically, P2G provides grid flexibility to support VRE integration …