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  • Membrane-free electrochemical production of acid and base solutions capable of processing ultramafic rocks. Nature communications Charnay, B. P., Chen, Y., Misleh, J. W., Wright, J. G., Agarwal, R. G., SauvĂ©, E. R., Toh, W. L., Surendranath, Y., Kanan, M. W. 2025; 16 (1): 9759

    Abstract

    Electrochemical production of acid and base from water enables their use as regenerable reagents in closed-loop processes, with attractive applications including CO2 capture or mineralization and low-temperature production of Ca(OH)2. Conventional systems utilize ion exchange membranes (IEMs) to inhibit H+/OH- recombination, which leads to high resistive losses that compromise energy efficiency and poor tolerance for polyvalent metal ions that complicates applications involving mineral resources. Here we use ion transport modeling to guide the design of a system that uses a simple porous separator instead of IEMs. Using H2 redox reactions for H+/OH- production, we demonstrate acid-base production at useful concentrations in the presence of polyvalent impurities with lower energy demand and higher current density than reported IEM-based systems. Cells can be stacked by combining H2 electrodes into a bipolar gas diffusion electrode, which recirculates H2 with near-unity efficiency. We show that the cell outputs extract alkalinity from olivine and serpentine as Mg(OH)2 and Mg3Si2O6(OH)2, which remove CO2 from ambient air to form Mg carbonates. These studies establish the principles for membrane-free electrochemical acid-base production, enabling closed-loop resource recovery and material processing powered by renewable electricity.

    View details for DOI 10.1038/s41467-025-64595-5

    View details for PubMedID 41193486

    View details for PubMedCentralID 10722509

  • 3D Lead-Organoselenide-Halide Perovskites and their Mixed-Chalcogenide and Mixed-Halide Alloys. Angewandte Chemie (International ed. in English) Karunadasa, H., Li, J., Wang, Y., Saha, S., Chen, Z., Hofmann, J., Misleh, J., Chapman, K. W., Reimer, J. A., Filip, M. R. 2024: e202408443

    Abstract

    We incorporate Se into the 3D halide perovskite framework using the zwitterionic ligand: SeCYS (+NH3(CH2)2Se-), which occupies both the X- and A+ sites in the prototypical ABX3 perovskite. The new organoselenide-halide perovskites: (SeCYS)PbX2 (X = Cl, Br) expand upon the recently discovered organosulfide-halide perovskites. Single-crystal X-ray diffraction and pair distribution function analysis reveal the average structures of the organoselenide-halide perovskites, whereas the local lead coordination environments and their distributions were probed through solid-state 77Se and 207Pb NMR, complemented by theoretical simulations. Density functional theory calculations illustrate that the band structures of (SeCYS)PbX2 largely resemble those of their S analogs, with similar band dispersion patterns, yet with a considerable bandgap decrease. Optical absorbance measurements indeed show bandgaps of 2.07 and 1.86 eV for (SeCYS)PbX2 with X = Cl and Br, respectively. We further demonstrate routes to alloying the halides (Cl, Br) and chalcogenides (S, Se) continuously tuning the bandgap from 1.86 to 2.31 eV-straddling the ideal range for tandem solar cells or visible-light photocatalysis. The comprehensive description of the average and local structures, and how they can fine-tune the bandgap and potential trap states, respectively, establishes the foundation for understanding this new perovskite family, which combines solid-state and organo-main-group chemistry.

    View details for DOI 10.1002/anie.202408443

    View details for PubMedID 38976771