No abstract

No abstract

Photoreduction of CO 2 provides an appealing way to alleviate the energy crisis and manage the global carbon balance but is limited by the high activation energy and the rate-limiting proton transfer. We now develop a dual-site strategy for high-efficiency CO 2 conversion through polarizing CO 2 molecules at pyridine N vacancies and accelerating the intermediate protonation by protonated pyridine N adjacent to nitrogen vacancies on polymeric carbon nitride. Our photocatalysts with atomic-level engineered active sites manifest a high CO production rate of 1835 μmol g À 1 h À 1 , 183 times higher than the pristine bulk carbon nitride. Theoretical prediction and experimental studies confirm that such excellent performance is attributed to the synergistic effect between vacant and protonated pyridine N in decreasing the formation energy of the key *COOH intermediates and the efficient electron transfer relay facilitated by the defect-induced shallow trap state and homogeneous charge mediators.

No abstract

No abstract

No abstract

Solar-driven photoelectrochemical (PEC) water splitting into hydrogen fuel is a promising avenue for renewable energy conversion to overcome energy crises and environmental concerns. Earth-abundant Si semiconductors with excellent light-harvesting capabilities are suitable photocathode candidates for the PEC hydrogen evolution reaction (HER), but suffer from intrinsic instability and sluggish kinetics. Extensive studies have demonstrated that surface/interface engineering can serve as an effective strategy for fabricating Si-based photocathodes with sufficient surface catalytic activity and facile interfacial carrier transport. In this Review, we first briefly introduce the current status of PEC HER using Si-based photocathodes and summarize their fabrication techniques. Subsequently, a systematic overview of recent achievements in surface/interface engineering of Si-based photocathodes is presented to illustrate their distinct roles in boosting the PEC-HER performance. Finally, the perspective views regarding the further development of practical Si-based photocathodes are discussed. This Review aims to promote an in-depth understanding and technical evaluation of surface/interface engineering strategies for efficient Si-based PEC HER.

An efficient water oxidation photocatalyst is imperative for the realization of artificial photosynthesis. Herein, a cooperative strategy is represented that enables 2D structure tailoring and lattice distortion engineering simultaneously over a BiVO4 photocatalyst for efficient visible‐light‐driven oxygen evolution reaction (OER). Specifically, the lattice distortion engineering is achieved through the introduction of a sodium (Na+) additive during the ion exchange process. Structural characterizations suggest the formation of ultrathin 2D monoclinic BiVO4 nanoflakes with shrank VO and elongated BiO bonds. Mechanistic investigations reveal the advantages of ultrathin 2D features for exposing more (010) active facets and shortening the required migration distance for charge carriers to reach the catalytic surface. More importantly, the lattice distortion effect is found to crucially govern the charge carrier dynamics and catalytic surface behavior of BiVO4 photocatalyst, endowing the optimized sample with an outstanding photocatalytic OER performance triggering up to 69.4% apparent quantum efficiency over Fe3+ sacrificial solution. These findings highlight the functional application of morphology and dimensional modification, as well as lattice distortion engineering in synthesizing superior monoclinic BiVO4 photocatalyst for efficient visible‐light‐driven water oxidation.