Electrochemical oxidative lignin cleavage and coupled 2‐furaldehyde reduction provide a promising approach for producing high‐value added products. However, developing efficient bifunctional electrocatalysts with noble‐metal‐like activity still remains a challenge. Here, an efficient electrochemical strategy is reported for the selective oxidative cleavage of Cα–Cβ bonds in lignin into aromatic monomers by tailoring the electronic structure through P‐doped CoMoO4 spinels (99% conversion, highest monomer selectivity of 56%). Additionally, the conversion and selectivity of 2‐furaldehyde reduction to 2‐methyl furan reach 87% and 73%, respectively. In situ Fourier transform infrared and density functional theory analysis reveal that an upward shift of the Ed upon P‐doping leads to an increase in the antibonding level, which facilitates the Cα–Cβ adsorption of the lignin model compounds, thereby enhancing the bifunctional electrocatalytic activity of the active site. This work explores the potential of a spinel as a bifunctional electrocatalyst for the oxidative cracking of lignin and the reductive conversion of small organic molecules to high‐value added chemicals via P‐anion modulation.
Infinite coordination-polymer particles (CPPs) are promising materials for solar energy conversion with high efficiency. However, the range of organic ligands that may be used to create CPPs is limited, as are strategies for modification, thereby hindering the applications of such material. In this paper, competitive evolution-morphological and structural change from Zn-based crystallites to amorphous particles is described. Controlled contribution of organic linkers selectively derived six Zn-CPPs with multivariate characters. Based on the diversity of these substructures, hollow zinc oxide particles were initially formed by selfpyrolysis of CPPs and effectively modified by ultrathin doped nanosheets. The obtained double-sided heterojunctions offer fully-covered active sites, bringing together efficient light-excited charge-transfer nanochannels, which exhibit an excellent solar H 2 -releasing activity (e.g., 4512.5 μmol h À 1 g À 1 ) and stable cyclability.Zn-based semiconductor-driven solar water splitting, regarded with redox innocent, low cost, and exceptional free charge transport properties, is an appealing process to achieve scalable hydrogen (H 2 ) generation. [1] Given the energetically uphill steps (Gibbs energy of + 237 kJ mol À 1 ) associated with the water splitting reaction, overcoming the well-known "thermodynamic contradictions" between optical absorption and redox potentials of the single Zn-based catalyst is an important challenge. [1c, 2] One of the effective
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