Search

CO2 reduction photocatalysts are favorable for obtaining renewable energy. Enriched active sites and effective photogenerated‐carriers separation are keys for improving CO2 photo‐reduction. A thulium (Tm) single atom tailoring strategy introducing carbon vacancies in porous tubular graphitic carbon nitride (g‐C3N4) surpassing the ever‐reported g‐C3N4 based photocatalysts, with 199.47 µmol g−1 h−1 CO yield, 96.8% CO selectivity, 0.84% apparent quantum efficiency and excellent photocatalytic stability, is implemented in this work. Results revealed that in‐plane Tm sites and interlayer‐bridged Tm‐N charge transfer channels significantly enhanced the aggregation/transfer of photogenerated electrons thus promoting CO2 adsorption/activation and contributing to *COOH intermediates formation. Meanwhile, Tm atoms and carbon vacancies both benefit for rich active sites and enhanced photogenerated‐charge separation, thus optimizing reaction pathway and leading to excellent CO2 photo‐reduction. This work not only provides guidelines for CO2 photo‐reduction catalysts design but also offers mechanistic insights into single‐atom based photocatalysts for solar fuel production. [ABSTRACT FROM AUTHOR]

Gel‐state polymer electrolytes with superior mechanical properties, self‐healing abilities and high Li+ transference numbers can be obtained by in situ polymerization of monomers with hydrogen‐bonding moieties. However, it is overlooked that the active hydrogen atoms in hydrogen‐bond donors experience displacement reactions with lithium metal in lithium metal batteries (LMBs), leading to corrosion of the lithium metal. Herein, it is discovered that the addition of hydrogen‐bond acceptors to hydrogen‐bond‐rich gel‐state electrolytes modulates the chemical activity of the active hydrogen atoms via the formation of hydrogen‐bonded intermolecular interactions. The characterizations reveal that the added hydrogen‐bond acceptors encapsulate the active hydrogen atoms to suppress the interfacial chemical corrosions of lithium metals, thereby enhancing the chemical stability of the polymer structure and interphase. With the employment of this strategy, a 1.1 Ah LiNi0.8Co0.1Mn0.1O2/Li metal pouch cell achieves stable cycling with 96.3 % capacity retention at 100 cycles. This new approach indicates a feasible path for achieving in situ polymerization of highly stable gel‐state‐based LMBs. [ABSTRACT FROM AUTHOR]

One‐unit‐cell, single‐crystal, hexagonal CuInP2S6 atomically thin sheets of≈0.81 nm in thickness was successfully synthesized for photocatalytic reduction of CO2. Exciting ethene (C2H4) as the main product was dominantly generated with the yield‐based selectivity reaching ≈56.4 %, and the electron‐based selectivity as high as ≈74.6 %. The tandem synergistic effect of charge‐enriched Cu−In dual sites confined on the lateral edge of the CuInP2S6 monolayer (ML) is mainly responsible for efficient conversion and high selectivity of the C2H4 product as the basal surface site of the ML, exposing S atoms, can not derive the CO2 photoreduction due to the high energy barrier for the proton‐coupled electron transfer of CO2 into *COOH. The marginal In site of the ML preeminently targets CO2 conversion to *CO under light illumination, and the *CO then migrates to the neighbor Cu sites for the subsequent C−C coupling reaction into C2H4 with thermodynamic and kinetic feasibility. Moreover, ultrathin structure of the ML also allows to shorten the transfer distance of charge carriers from the interior onto the surface, thus inhibiting electron‐hole recombination and enabling more electrons to survive and accumulate on the exposed active sites for CO2 reduction. [ABSTRACT FROM AUTHOR]

The establishment of green and environmental friendly sunlight‐driven organic reactions has received increasing attention since the 21st century. By virtue of their functional designability, micromesoporous structure, and thermal/chemical stability, porous organic polymers (POPs) have exhibited enormous promise in photocatalytic organic reactions as ideal potential alternatives to conventional small molecule and inorganic semiconductor catalysts. In particular, amorphous POPs are simplified in terms of preparation conditions and process flow. Herein, various amorphous POP materials based on polymers of intrinsic microporosity, hypercrosslinked polymers, conjugated microporous polymers, and porous aromatic frameworks are reviewed, while typical synthetic strategies are briefly introduced. It also highlights an overview of the research progress in photocatalytic oxidation, coupling, reduction, cycloaddition, and polymerization reactions at home and abroad in recent years. Finally, the challenges and prospects for future research on amorphous POPs are presented. [ABSTRACT FROM AUTHOR]