Catalyst and Catalysis Co-Exploration in Methane Utilization

Abstract Conventional catalyst development is typically confined to reaction-centric approaches, in which catalyst performance is evaluated under fixed feed compositions targeting a single desired product. Such strategies overlook the complexity of multicomponent reaction environments, where multiple competing pathways can emerge. Here, we present a high-throughput approach that enables the simultaneous exploration of catalyst composition and reaction conditions, using methane conversion as a representative system. Methane transformation was systematically investigated over a library of 200 catalysts across a broad CH4−O2−CO2 feed compositional space, without imposing predefined reaction targets or stoichiometric constraints. Product formation was monitored using unbiased full mass-scan analysis, allowing hydrocarbons, syngas components, and minor products to emerge directly from the data. Moving beyond conventional benchmarks, optimal performance frequently arises at feed compositions that deviate significantly from the stoichiometric ratios of established methane reactions. Expanding the accessible reaction space not only enhances attainable yields but also reveals high-performing catalysts that would remain unrecognized under fixed-condition evaluation. The results further demonstrate that catalytic performance arises from coupled catalyst–condition interactions, rather than intrinsic material properties assessed at a single feed condition.