Ensembles of Photosynthetic Nanoreactors

Our scientific mission is to understand, predict, and control the activity, selectivity, and stability of solar water splitting nanoreactors in isolation and as ensembles.

EPN Overview Figure

EPN builds “nanoreactors,” that is, very small reactors around 100,000 times smaller than a grain of rice. The foundation of each nanoreactor is a light absorbing semiconductor, a material that can absorb sunlight and convert it into electricity. This light absorber is then surrounded by a coating that acts as a guard, only allowing the proper chemicals to pass through. To complete these nanoreactors, they are combined with catalysts, the chemicals that actually facilitate hydrogen generation. One chemical process builds billions upon billions of these nanoreactors, which added together, produces commercially viable hydrogen from water.  Written by Olivia Bird, EPN Graduate Student

Research Goals and Approaches

  • Extend photocarrier lifetimes (>10x radiative “limit”) and control their dynamics during infrequent photon absorption events
  • Enhance charge-separation yields (>50%) and redox selectivity (>90%), and therefore stability, under conditions of low-flux carrier transport (i.e. low current density)
  • Program ensembles of artificial photosystems for large solar-to-hydrogen (STH) efficiencies (>10% STH)

To achieve these goals, EPN is developing powerful new and synergistic experimental and theoretical capabilities in nanomaterials synthesis, multiphysics modeling, and coupled correlative microscopies and spectroscopies. Results across a multitude of length and time scales teach physicochemical principles that dictate the behavior of ensembles of nanoreactors. This information serves as inputs to inverse design analyses, whose outputs guide optimization through a codesign feedback loop for bottom-up synthesis of multicomponent interphase coatings.


Electronic Selectivity

(i) Use operando correlative multimodal microscopies to reveal charge separation mechanisms and (ii) Determine the influence of discrete photoinduced events on steady-state water splitting reactivity

Reactant Accumulation

(i) Extend photogenerated charge-carrier lifetimes and (ii) Control species accumulation at atomically precise reaction centers during infrequent photon absorption

Chemical Selectivity

(i) Understand in atomistic detail the function of encapsulated molecular reaction centers and (ii) Codesign spatially distinct interphases for species-specific permeabilities and stabilities at low flux

Ensemble Effects

(i) Experimentally validate interparticle interactions mediated by light and matter and (ii) Program desired physicochemical properties, guided by simulations bridging microenvironments

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