• Energy Research

AbstractSolar fuels offer a promising approach to provide sustainable fuels by harnessing sunlight1,2. Following a decade of advancement, Cu2O photocathodes are capable of delivering a performance comparable to that of photoelectrodes with established photovoltaic materials3–5. However, considerable bulk charge carrier recombination that is poorly understood still limits further advances in performance6. Here we demonstrate performance of Cu2O photocathodes beyond the state-of-the-art by exploiting a new conceptual understanding of carrier recombination and transport in single-crystal Cu2O thin films. Using ambient liquid-phase epitaxy, we present a new method to grow single-crystal Cu2O samples with three crystal orientations. Broadband femtosecond transient reflection spectroscopy measurements were used to quantify anisotropic optoelectronic properties, through which the carrier mobility along the [111] direction was found to be an order of magnitude higher than those along other orientations. Driven by these findings, we developed a polycrystalline Cu2O photocathode with an extraordinarily pure (111) orientation and (111) terminating facets using a simple and low-cost method, which delivers 7 mA cm−2 current density (more than 70% improvement compared to that of state-of-the-art electrodeposited devices) at 0.5 V versus a reversible hydrogen electrode under air mass 1.5 G illumination, and stable operation over at least 120 h.

Summary: Due to the highly complex polyphenolic structure of lignin, depolymerization without a prior chemical treatment is challenging, and new catalysts are required. Atomically dispersed catalysts are able to maximize the atomic efficiency of noble metals, simultaneously providing an alternative strategy to tune the activity and selectivity by alloying with other abundant metal supports. Here, we report a highly active and selective catalyst comprising monodispersed (single) Pt atoms on Ni nanoparticles supported on carbon (denoted as Pt1Ni/C, where Pt1 represents single Pt atoms), designed for the reductive depolymerization of lignin. Selectivity toward 4-n-propylsyringol and 4-n-propylguaiacol exceeds 90%. The activity and selectivity of the Pt1Ni/C catalyst in the reductive depolymerization of lignin may be attributed to synergistic effects between the Ni nanoparticles and the single Pt atoms.