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Aerobic oxidation by using molecular oxygen (O2) as the oxidant is highly attractive, in which activating O2 to reactive oxygen species (ROS) is a prerequisite. Although some progress has been achieved in regulating ROS by heterogeneous catalysts, the strategies to efficiently control ROS in aerobic oxidation are still urgently desired. Herein, grain boundaries (GBs) in metal oxides are discovered to be able to facilely regulate ROS. Impressively, MoO3 nanocrystals with high density of GBs (MoO3‐600) deliver a mass activity of 83 mmol g‐1 h‐1 in aerobic oxidation of benzyl alcohol, 7 and 8 times as high as that of MoO3 nanoparticles without GBs and Pt/C, respectively. In addition, the selectivity of benzoic acid is 100% during whole reaction process over MoO3‐600. Mechanistic studies reveal that the oxygen atoms at GBs in MoO3‐600 are highly active to form ∙OH radicals with the generation of oxygen vacancies, while the oxygen vacancies are replenished by O2. The reaction path directly contributes to the excellent catalytic performance. [ABSTRACT FROM AUTHOR]

The standard of clinical care of most malignant solid cancers is surgery, followed by postsurgical adjuvant therapy, but microtumor lesions left behind after surgery and invisible distant metastases are the major reasons for treatment failure. Here, we report an integrated strategy combining surface-enhanced Raman spectroscopy (SERS) surgical navigation with postsurgical immunotherapy elicited by near-infrared II photothermal treatment and programmed death-1 antibody. The SERS surgical navigation is principally based on the multifunctional optical probes (namely, MATRA probes) integrating with T 1 -weighted magnetic resonance (MR) imaging, photothermal effect and Raman spectroscopic detection. We demonstrate in a 4T1 breast tumor mouse model that the pre-surgical MR/SERS dual-modal imaging is capable of providing comprehensive tumor information, and intraoperative SERS detection allows accurately delineating the tumor margins and guiding the surgical resection in real time with the least residual microscopic foci. We verify that the postsurgical immunotherapy effectively eradicates those local microtumor lesions and invisible distant metastases, greatly inhibiting the postsurgical cancer recurrence and distant metastasis.