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Abstract: Crystalline and porous covalent organic frameworks (COFs) and metal‐organic frameworks (MOFs) materials have attracted enormous attention in the field of photocatalytic H2 evolution due to their long‐range order structures, large surface areas, outstanding visible light absorbance, and tunable band gaps. In this work, we successfully integrated two‐dimensional (2D) COF with stable MOF. By covalently anchoring NH2‐UiO‐66 onto the surface of TpPa‐1‐COF, a new type of MOF/COF hybrid materials with high surface area, porous framework, and high crystallinity was synthesized. The resulting hierarchical porous hybrid materials show efficient photocatalytic H2 evolution under visible light irradiation. Especially, NH2‐UiO‐66/TpPa‐1‐COF (4:6) exhibits the maximum photocatalytic H2 evolution rate of 23.41 mmol g−1 h−1 (with the TOF of 402.36 h−1), which is approximately 20 times higher than that of the parent TpPa‐1‐COF and the best performance photocatalyst for H2 evolution among various MOF‐ and COF‐based photocatalysts. [ABSTRACT FROM AUTHOR]

The design of highly stable, selective and efficient electrocatalysts for CO2 reduction reaction is desirable while largely unmet. In this work, a series of precisely designed polyoxometalate-metalloporphyrin organic frameworks are developed. Noted that the integration of {ε-PMo8VMo4VIO40Zn4} cluster and metalloporphyrin endows these polyoxometalate-metalloporphyrin organic frameworks greatly advantages in terms of electron collecting and donating, electron migration and electrocatalytic active component in the CO2 reduction reaction. Thus-obtained catalysts finally present excellent performances and the mechanisms of catalysis processes are discussed and revealed by density functional theory calculations. Most importantly, Co-PMOF exhibits remarkable faradaic efficiency ( > 94%) over a wide potential range (−0.8 to −1.0 V). Its best faradaic efficiency can reach up to 99% (highest in reported metal-organic frameworks) and it exhibits a high turnover frequency of 1656 h−1 and excellent catalysis stability ( > 36 h). While CO2 reduction provides a way to remove carbon from the atmosphere, it is challenging to design effective, selective materials for this process. Here, authors construct metal-organic frameworks from polyoxometalates and porphryins to direct electron flow and improve CO2 reduction efficiencies. [ABSTRACT FROM AUTHOR]

The electrochemical reduction of carbon dioxide (CO 2 ) to ethylene creates a carbon-neutral approach to converting carbon dioxide into intermittent renewable electricity. Exploring efficient electrocatalysts with potentially high ethylene selectivity is extremely desirable, but still challenging. In this report, a laboratory-designed catalyst HKUST-1@Cu 2 O/PTFE-1 is prepared, in which the high specific surface area of the composites with improved CO 2 adsorption and the abundance of active sites contribute to the increased electrocatalytic activity. Furthermore, the hydrophobic interface constructed by the hydrophobic material polytetrafluoroethylene (PTFE) effectively inhibits the occurrence of hydrogen evolution reactions, providing a significant improvement in the efficiency of CO 2 electroreduction. The distinctive structures result in the remarkable hydrocarbon fuels generation with high Faraday efficiency (FE) of 67.41%, particularly for ethylene with FE of 46.08% (-1.0 V vs RHE). The superior performance of the catalyst is verified by DFT calculation with lower Gibbs free energy of the intermediate interactions with improved proton migration and selectivity to emerge the polycarbon（C 2+ ） product. In this work, a promising and effective strategy is presented to configure MOF-based materials with tailored hydrophobic interface, high adsorption selectivity and more exposed active sites for enhancing the efficiency of the electroreduction of CO 2 to C 2+ products with high added value., (© 2023 Wiley‐VCH GmbH.)

Crystalline and porous covalent organic frameworks (COFs) and metal-organic frameworks (MOFs) materials have attracted enormous attention in the field of photocatalytic H 2 evolution due to their long-range order structures, large surface areas, outstanding visible light absorbance, and tunable band gaps. In this work, we successfully integrated two-dimensional (2D) COF with stable MOF. By covalently anchoring NH 2 -UiO-66 onto the surface of TpPa-1-COF, a new type of MOF/COF hybrid materials with high surface area, porous framework, and high crystallinity was synthesized. The resulting hierarchical porous hybrid materials show efficient photocatalytic H 2 evolution under visible light irradiation. Especially, NH 2 -UiO-66/TpPa-1-COF (4:6) exhibits the maximum photocatalytic H 2 evolution rate of 23.41 mmol g -1  h -1 (with the TOF of 402.36 h -1 ), which is approximately 20 times higher than that of the parent TpPa-1-COF and the best performance photocatalyst for H 2 evolution among various MOF- and COF-based photocatalysts., (© 2018 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.)