Porous covalent organic frameworks (COFs) are promising materials used for separation and purification during environmental remediation. This critical review focuses on two key aspects. First, it critically examines strategies to improve COF design and structure and evaluates their impact on separation performance. Second, engineering approaches for enhancing the interactions between COF-based adsorbents and metals for enhanced separation and capture are elucidated. The latest body of research on separating metals (e.g., Li, K, Sr, Hg, Cd, Pb, Cr, Au, Ag, Pd, and U) using COF-based adsorbents is discussed to understand the factors that influence their performance. However, it is to be noted that COF-based adsorbents are still in their infancy and remain largley unexplored, mainly hindered by synthetic complexities and suboptimal crystalline structures. This highlights the need for further research and development to fully unlock the excellent potential of COFs for metal separation applications, particularly in environmental and energy applications.

In our pursuit of an efficient catalyst for ammonia production, we developed ruthenium (Ru)-based single atom alloy catalysts on a layered double hydroxide-derived support. The extended X-ray absorption fine structure studies provided evidence of single Ru atoms as a Fe-Ru alloy. High-resolution transmission electron microscopy showcased a larger particle size with higher Ru loading, emphasizing the role of Ru site geometry in catalytic activity. The MgFeOx-0.1Ru catalyst, with optimal Ru dispersion and smaller Fe-Ru particle size (1.6 nm), outperformed other catalysts in NH3 synthesis and demonstrated exceptional stability. Remarkably, the catalyst with 0.1 wt% Ru exhibited superior performance, achieving an exceptional NH3 formation rate of 17,897 µmol g−1 h−1 (at 400 °C, 5 MPa, and Weight hourly space velocity (WHSV) of 50,000 mL g−1 h−1) along with maintaining a consistent NH3 synthesis rate of 7,217 µmol g−1 h−1 (at 400 °C, WHSV of 10,000 mL g−1 h−1, and 5 MPa), for a notable duration of 150 h. Our first-principles calculations show that Ru weakened the binding of both molecular and atomic nitrogen on the catalyst's surface, facilitating the desorption of N-intermediates. The optimized MgFeOx-0.1Ru catalyst composition with characteristics such as small Fe-Ru alloy particle size and the presence of all active Ru sites on the surface improves lifetime, reducing costs and marking a significant stride towards sustainable and economically viable NH3 production.

Electrochemical water splitting and energy storage are key for a sustainable energy future, despite the challenges related to undesirable overpotentials and high voltage requirements. Herein, we introduce a synergistic approach between a low overpotential hydrogen evolution reaction (HER) and a low voltage zinc-air/iodine battery (ZAIB) by coupling with iodide oxidation half reactions. By developing a Pt/Co3O4 electrocatalyst in two steps and with under 2% Pt loading, we achieve an unprecedented low full cell potential for hydrogen generation at 0.574 V, exhibiting an ultra-high reduction of energy consumption of 64.7%. The Pt/Co3O4 electrode also enables ZAIB to record a power density of 154 mW cm−2 at an ultra-low charging potential of 1.68 V. Mechanistic studies and DFT calculations of the novel electrode confirm an electron rich Pt-Co interface and favorable Pt-I interactions, facilitating both HER and IOR reactions. Our design provides critical technology for potential large-scale renewable energy projects.

Supported single-atom catalysts (SACs) are promising in heterogeneous catalysis because of their atom economy, unusual transformations, and mechanistic clarity. The metal SAs loading, however, limits the catalytic efficiency. Herein, an in situ pre-metallated monomer-based preparation strategy is shown to achieve ultrahigh Au SAs loading in catalyst formations. The polymerization of single-atom loaded monomers yield a new porous aromatic framework (PAF-164) with Au SAs loading up to a record high 45.3 wt.%. SACs of Au-PAFs exhibit excellent photocatalytic activity in hydrogen (H2) evolution, and the H2 evolution rate of Au100%-SAs-PAF-164 can reach 4.82 mmol g−1 h−1 with great recyclability.

Asymmetric catalysis for enantioselective intramolecular hydroamination of alkenes is a critical method in the construction of enantioenriched nitrogen-containing rings, often prevalent in biologically active compounds and natural products. Herein, we demonstrate a facile enantioselective intramolecular hydroamination of alkenes for the synthesis of chiral pyrrolidine, piperidine, and indoline moieties, using a manganese (II) chiral aprotic cyclic urea catalyst. The cyclic ligand hinders the inversion of the N atom of the urea and effectively discriminate between the enantiomers of substrates. High-resolution mass spectrometry, deuterium labeling experiments, and molecular orbital energy analysis clearly reveal the intermediates and mechanism of the transformation. As a key step, oxygen coordination by chiral aprotic urea presents a robust control over the asymmetric intra-HA reaction through the involvement of a convergent assembly of two vital intermediates (Mn-N and C-Mn-Br), providing access to chiral cyclic amine systems in high yields with excellent enantioselectivity.