ConspectusModern catalysis has traditionally focused on the optimization of isolated active sites; however, industrial-scale chemical manufacturing relies on the integration of reaction, transfer, separation, and feedback operations. The disconnection between these two disciplines─catalysis and process engineering─creates a fundamental gap between molecular precision and process efficiency. Bridging this gap requires reimagining the catalyst not as a static reactive surface, but as a nano miniaturized chemical process, where sequential unit operations are spatially and kinetically coordinated within a single material framework. Consequently, achieving such process intensification at the catalytic scale represents one of the frontier challenges in sustainable chemistry and materials design.Bifunctional and multifunctional catalysts provide an effective platform for this translation of process logic into nanoscale architectures. By assigning different catalytic domains to distinct elementary operations─activation, transfer, and transformation─these systems can emulate the functional synergy of macroscopic chemical plants within confined spatial dimensions. Conceptually, this strategy parallels reaction-transfer-separation-rereaction in chemical-engineering, compressing these steps into a single composite catalyst. The resulting complexity, however, introduces new scientific questions: how can multiple reaction domains communicate, balance kinetics, and sustain cooperative efficiency while preserving thermodynamic directionality?This Account summarizes our efforts to address these challenges through the rational design of process-coordinated COx conversion catalysts. Three representative strategies are highlighted: (i) engineering the activation-hydrogenation unit through atomic-level dispersion and Fe-Fe bond-length tuning to optimize upstream reactivity; (ii) regulating intermediate transfer using a bioinspired catalytic shunt mechanism that controls adsorption strength and pathway branching; and (iii) achieving kinetic synchronization between domains via valence-state modulation to match intermediate formation and transformation rates. Together, these strategies define an integrated framework for nanoscale process intensification, transforming the catalyst into a self-regulating microreactor that mimics the logic of chemical process units. Looking forward, the concept can be extended to hierarchically coupled, dynamically adaptive systems where artificial intelligence and machine-learning-assisted design enable data-driven discovery, real-time feedback, and autonomous optimization─ushering in intelligent catalysts that unify reaction and process engineering at the molecular scale.
Tian et al. (Mon,) studied this question.