Publications

The solar-driven reduction of carbon dioxide to value-added chemical fuels is a longstanding challenge in the fields of catalysis, energy science, and green chemistry. In order to develop effective CO2 fixation, several key considerations must be balanced, including (1) catalyst selectivity for promoting CO2 reduction over competing hydrogen generation from proton reduction, (2) visible-light harvesting that matches the solar spectrum, and (3) the use of cheap and earth-abundant catalytic components. In this report, we present the synthesis and characterization of a new family of earth-abundant nickel complexes supported by N-heterocyclic carbene-amine ligands that exhibit high selectivity and activity for the electrocatalytic and photocatalytic conversion of CO2 to CO. Systematic changes in the carbene and amine donors of the ligand have been surveyed, and [Ni((Pr)bimiq1)](2+) (1c, where (Pr)bimiq1 = bis(3-(imidazolyl)isoquinolinyl)propane) emerges as a catalyst for electrochemical reduction of CO2 with the lowest cathodic onset potential (E(cat) = -1.2 V vs SCE). Using this earth-abundant catalyst with Ir(ppy)3 (where ppy = 2-phenylpyridine) and an electron donor, we have developed a visible-light photoredox system for the catalytic conversion of CO2 to CO that proceeds with high selectivity and activity and achieves turnover numbers and turnover frequencies reaching 98,000 and 3.9 s(-1), respectively. Further studies reveal that the overall efficiency of this solar-to-fuel cycle may be limited by the formation of the active Ni catalyst and/or the chemical reduction of CO2 to CO at the reduced nickel center and provide a starting point for improved photoredox systems for sustainable carbon-neutral energy conversion.

An entry from the Cambridge Structural Database, the world’s repository for small molecule crystal structures. The entry contains experimental data from a crystal diffraction study. The deposited dataset for this entry is freely available from the CCDC and typically includes 3D coordinates, cell parameters, space group, experimental conditions and quality measures.

An entry from the Cambridge Structural Database, the world’s repository for small molecule crystal structures. The entry contains experimental data from a crystal diffraction study. The deposited dataset for this entry is freely available from the CCDC and typically includes 3D coordinates, cell parameters, space group, experimental conditions and quality measures.

Mrk 501 is a prototypical high-synchrotron-peaked blazar (HBL) and serves as one of the primary targets for the {\it Imaging X-ray Polarimetry Explorer} ({\it IXPE}). In this study, we report X-ray polarization measurements of Mrk 501 based on six {\it IXPE} observations. The detection of X-ray polarization at a confidence level exceeding 99\% is achieved in four out of the six observations conducted across the entire energy range (2--8 keV) of {\it IXPE}. The maximum polarization degree ($Π_{\rm X}$) is measured to be $15.8\%\pm2.8\%$, accompanied by a polarization angle ($ψ_{\rm X}$) of $98.0°\pm5.1°$ at a confidence level of $5.6 σ$. During the remaining two observations, only an upper limit of $Π_{\rm X}<$12\% could be derived at the 99\% confidence level. No temporal variability in polarization is observed throughout all six {\it IXPE} observations for Mrk 501. A discernible trend of energy-dependent variation in the polarization degree is detected in optical spectropolarimetry; however, no analogous indication is observed in $Π_{\rm X}$. The chromatic behavior of $Π$ and the consistent values of $ψ$ across different frequencies from X-rays to radio waves, along with the agreement between $ψ$ and jet position angle, strongly support the interpretation of the energy-stratified model with shock-accelerated particles in the jet of Mrk 501. Additionally, the possibility of the presence of a global helical magnetic field in the jet of Mrk 501 is discussed.

An entry from the Cambridge Structural Database, the world’s repository for small molecule crystal structures. The entry contains experimental data from a crystal diffraction study. The deposited dataset for this entry is freely available from the CCDC and typically includes 3D coordinates, cell parameters, space group, experimental conditions and quality measures.

A solution-phase route for the preparation of single-crystalline iron phosphide nanorods and nanowires is reported. We have shown that the mixture of trioctylphosphine oxide (TOPO) and trioctylphosphine (TOP), which are commonly used as the solvents for semiconductor nanocrystal synthesis, is not entirely inert. In the current process, TOP, serving as phosphor source, reacts with Fe precursors to form FeP nanostructures with large aspect ratios. In addition, the experimental results show that both TOP and TOPO are necessary for the formation of FeP nanowires and their ratio appears to control the morphology of the produced FeP structures. A possible growth mechanism is discussed.