No abstract

Poly (3,4-ethylene dioxythiophene) (PEDOT) is an electrically conductive polymer that shows various promising applications in flexible electronics. However, previous studies have mostly focused on enhancing the conductivity, while ignoring the design and development of porous PEDOT materials. Herein, we report a novel and sustainable strategy of utilizing a deep eutectic solvent of ferric chloride hexahydrate/acetamide to guide the interfacecontrolled polymerization of PEDOT at room temperature. The obtained PEDOT material has its unique features of high porosity of 70.61%, high specific surface area of >58 m 2 /g, and ideal electrical conductivity of 6500 S/m, resulting in a wide voltage window of up to 1.2 V. Notably, this porous PEDOT can be easily formulated into printable electronic ink with controllable rheological properties, process ability, and recyclability, exhibiting the outstanding energy storage behavior in wearable electronics. This study reports an effective, green approach for the development of porous PEDOT materials and printable flexible devices.

Phosphorus‐doped carbon materials are promising alternatives to noble metal‐based catalysts for the highly selective oxidation of benzyl alcohol to benzaldehyde, but it is challenging to achieve high loadings of high‐activity P dopants in metal‐free catalysts. Here, the preparation of high‐loading and well‐dispersed P atoms confined to the surfaces of cellulose‐derived carbon via a dissolving‐doping strategy is reported. In this method, cellulose is dissolved in phosphoric acid to generate a cellulose‐phosphoric supramolecular collosol, which is then directly carbonized. The as‐prepared carbon possesses a high specific surface area of 1491 cm3 g−1 and a high P content of 8.8 wt%. The P‐doped nanoporous carbon shows a superior catalytic activity and cyclic stability toward benzyl alcohol oxidation, with a high turnover frequency of 3.5 × 10−3 mol g−1 h−1 and a low activation energy of 35.6 kJ mol−1. Experimental results and theoretical calculations demonstrate that the graphitic C3PO species is the leading catalytic active center in this material. This study provides a novel strategy to prepare P dopants in nanoporous carbon materials with excellent catalytic performance.

An in‐depth understanding of the electronic structures of catalytically active centers and their surrounding vicinity is key to clarifying the structure–activity relationship, and thus enabling the design and development of novel metal‐free carbon‐based materials with desired catalytic performance. In this study, boron atoms are introduced into phosphorus‐doped nanoporous carbon via an efficient strategy, so that the resulting material delivers better catalytic performance. The doped B atoms alter the electronic structures of active sites and cause the adjacent C atoms to act as additional active sites that catalyze the reaction. The B/P co‐doped nanoporous carbon shows remarkable catalytic performance for benzyl alcohol oxidation, achieving high yield (over 91% within 2 h) and selectivity (95%), as well as low activation energy (32.2 kJ mol−1). Moreover, both the conversion and selectivity remain above 90% after five reaction cycles. Density functional theory calculations indicate that the introduction of B to P‐doped nanoporous carbon significantly increases the electron density at the Fermi level and that the oxidation of benzyl alcohol occurs via a different reaction pathway with a very low energy barrier. These findings provide important insights into the relationship between catalytic performance and electronic structure for the design of dual‐doped metal‐free carbon catalysts.

Cellulose with numerous hydroxyl groups and electronegative atoms can form extensive hydrogen bonds, which are nonnegligible recalcitrants to dissolution and to further utilizations. Herein, an indepth understanding of the interactions...