科研成果 by Type: 期刊论文

Alquimia v1.0 is a generic interface to geochemical solvers that facilitates development of multiphysics simulators by enabling code coupling, prototyping and benchmarking. The interface enforces the function arguments and their types for setting up, solving, serving up output data and carrying out other common auxiliary tasks while providing a set of structures for data transfer between the multiphysics code driving the simulation and the geochemical solver. Alquimia relies on a single-cell approach that permits operator splitting coupling and parallel computation. We describe the implementation in Alquimia of two widely used open-source codes that perform geochemical calculations: PFLOTRAN and CrunchFlow. We then exemplify its use for the implementation and simulation of reactive transport in porous media by two open-source flow and transport simulators: Amanzi and ParFlow. We also demonstrate its use for the simulation of coupled processes in novel multiphysics applications including the effect of multiphase flow on reaction rates at the pore scale with OpenFOAM, the role of complex biogeochemical processes in land surface models such as the E3SM Land Model (ELM) and the impact of surface–subsurface hydrological interactions on hydrogeochemical export from watersheds with the Advanced Terrestrial Simulator (ATS). These applications make it apparent that the availability of a well-defined yet flexible interface has the potential to improve the software development workflow, freeing up resources to focus on advances in process models and mechanistic understanding of coupled problems.

Abstract Subsurface gas storage is crucial for achieving a sustainable energy future, as it helps to reduce CO2 emissions and facilitates the provision of renewable energy sources. The confinement effect of the nanopores in caprock induces distinctive thermophysical properties and fluid dynamics. In this paper, we present a multi-scale study to characterize the subsurface transport of CO2, CH4, and H2. A nanoscale-extended volume-translated Cubic-Plus-Association equation of state was developed and incorporated in a field-scale numerical simulation, based on a full reservoir-caprock suite model. Results suggest that in the transition from nanoscale to bulk-scale, gas solubility in water decreases while phase density and interfacial tension increase. For the first time, a power law relationship was identified between the capillary pressure within nanopores and the pore size. Controlled by buoyancy, viscous force and capillary pressure, gases transport vertically and horizontally in reservoir and caprock. H2 has the maximum potential to move upward and the lowest areal sweep efficiency; in short term, CH4 is more prone to upward migration compared to CO2, while in long term, CH4 and CO2 perform comparably. Thicker caprock and larger caprock pore size generally bring greater upward inclination. Gases penetrate the caprock when CH4 is stored with a caprock thickness smaller than 28 m or H2 is stored with a caprock pore size of 2–10 nm or larger than 100 nm. This study sheds light on the fluid properties and dynamics in nanoconfined environment and is expected to contribute to the safe implementation of gigatonne scale subsurface gas storage.

The catalytic partial oxidation of methane (POM) presents a promising technology for synthesizing syngas. However, it faces severe over-oxidation over catalyst surface. Attempts to modify metal surfaces by incorporating a secondary metal towards C–H bond activation of CH4 with moderate O* adsorption have remained the subject of intense research yet challenging. Herein, we report that high catalytic performance for POM can be achieved by the regulation of O* occupation in the atomically dispersed (AD) MoNi alloy, with over 95% CH4 conversion and 97% syngas selectivity at 800 °C. The combination of ex-situ/in-situ characterizations, kinetic analysis and DFT (density functional theory) calculations reveal thatMo-Ni dual sites inADMoNi alloy afford the declined O2 poisoning on Ni sites with rarely weaken CH4 activation for partial oxidation pathway following the combustion reforming reaction (CRR) mechanism. These results underscore the effectiveness ofCH4 turnovers by the design of atomically dispersed alloys with tunable O* adsorption