Intrinsic Oxygen Vacancies Research Articles

Tailoring Intrinsic Oxygen Vacancies in P3-Type Na0.66Mn0.66Mg0.33O1.93 to Enhance Oxygen Redox Activity.

Integrating oxygen redox reactions with transition metal redox reactions offers a promising strategy to double or triple the energy density for large-capacity battery cathodes. In this study, we have introduced intrinsic oxygen vacancies (VO) into a P3 layered cathode to modulate the electronic structure of O atoms and enhance oxygen redox activity. Rietveld-refined X-ray diffraction (XRD), X-ray absorption spectroscopy (XAS), and X-ray photoelectron spectroscopy confirm the successful creation of VO in Na0.66Mn0.66Mg0.33O1.93 (OV-NMM). Density functional theory (DFT) calculations reveal that VO in OV-NMM positively enhances the antibonding interaction between Mn and O, directing excess electrons from O holes toward adjacent Mn t2g and O 2p orbitals. This modification significantly improves the reversibility and accelerates Na+ transport kinetics for O2-/O- redox reactions. Ex situ synthon-based XRD demonstrates that VO effectively eliminates the O3 phase, reduces Mg2+ migration, and suppresses irreversible structural changes. XAS of Mn K-edge and O K-edge further illustrate the advantageous role of oxygen vacancies in facilitating oxygen redox reactions. These findings highlight the potential of defect engineering, particularly VO, to boost anionic redox activity for high-capacity energy storage applications.

Oxygen vacancies-enriched spent lithium-ion battery cathode materials loaded catalytic membrane for effective peracetic acid activation and organic pollutants degradation

Advanced oxidation processes combined with membrane filtration technique offer a promising approach for pollution mitigation and catalyst recovery. Herein, a waste ternary lithium-ion battery cathode material of LiNixCoyMnzO2 (LNCM) loaded polytetrafluoroethylene (PTFE) membrane was synthesized for peracetic acid (PAA) activation (LNCM-PTFE/PAA) and 2,4,6-trichlorophenol (TCP) degradation. Such a novel membrane, with a catalyst loading of 10 mg (0.796 mg/cm2) of LNCM achieved 96.4 % removal of TCP (2 mg/L) within 20 min in neutral pH. The redox cycles of surface metals (such as Co3+/Co2+, Ni3+/Ni2+, and Mn4+/Mn3+/Mn2+) in spent LNCM efficiently enhance charge transfer and mediated PAA activation. And intrinsic oxygen vacancies in LNCM facilitated PAA adsorption and its cleavage. The resulting carbon-centered radicals (R-C•, CH3C(O)OO•) and 1O2 are identified as the primary reactive species that collaboratively participate in TCP degradation. Quantitative structure-activity relationship analysis demonstrated a substantial reduction in product toxicity. The successful practical application of the LNCM-PTFE/PAA membrane was exemplified by treating chlorophenol industrial wastewater. This study presents a new LNCM-PTFE/PAA catalytic membrane for high-efficiency water treatment and a novel perspective for green utilization of waste LNCM.

Stable Long-Persistent Luminescence from Self-Activated CaSb2O6 Induced by Intrinsic Defects.

Long-persistent luminescence (LPL) materials have attracted intensive attention due to their fascinating emission after excitation. However, current LPL materials typically depend on external doping to introduce traps or emitting centers, resulting in a complex synthesis and controllability. For the first time, we develop another category of undoped LPL materials based on antimonate CaSb2O6, which exhibits blue LPL for over 8000 s. Both experimental and theoretical evidence indicate that excitons are trapped by intrinsic oxygen vacancies. Then, they are detrapped and recombine through singlet and triplet emission of Sb3+ to form LPL. Moreover, CaSb2O6 maintains approximately 100% of its initial LPL performance and structural integrity even after being treated under 1000 °C, UV irradiation, and extreme conditions (pH = 1 or 13). This study highlights the significant potential of antimonates as robust and versatile luminescent materials.

Abundant interfacial and intrinsic oxygen vacancies enabling small nickel/ceria nanocrystal efficient CO2 methanation

Smaller nano-sizes typically result in supported catalysts with abundant interfacial and intrinsic oxygen vacancies for better adsorption and activation of small molecules, including CO2, leading to improved efficiency of CO2 methanation. Here, Ni/CeO2-S with the smaller nano-size of around 4.2 nm is used to catalyze CO2 methanation, which exhibits significantly enhanced activity compared to larger nano-sized Ni/CeO2-L catalyst, even surpassing the most majority of previously reported catalysts using CeO2 as the support or Ni as the active metal. The coexistence of interfacial defects and intrinsic oxygen vacancies allows for enhanced adsorption and activation of CO2 molecules as well as H spillover, resulting in such improved CO2 methanation. In-situ DRIFTS demonstrate a nearly sole Formate pathway on Ni/CeO2-S for efficient CO2 hydrogenation. This research provides valuable insights into the reaction mechanism over a small nanosize supported catalyst.

Boosting electrochemical ammonia synthesis via dynamic nitrogen carriers coupled with electron-rich Lewis acidic sites on TiO2−x nanofiber

In light of the high energy consumption and substantial carbon emissions associated with traditional NH3 production based on the Haber–Bosch process, the aqueous electrochemical nitrogen reduction reaction (NRR) offers a clean and sustainable alternative production route. Nevertheless, activating the NN bonds at room temperature is challenging due to the high bond energy, severely hindering the development and commercialization of the electrochemical NRR. Herein, we report a synergistic strategy for achieving efficient N2 activation at ambient conditions that combines electrolyte engineering with catalytic site-modulated TiO2−x nanofiber electrocatalysts. The synthesized TiO2−x nanofiber electrocatalysts contained abundant intrinsic oxygen vacancies and were further modified with hydroxyl groups to create electron-rich Lewis acidic Ti sites. Additionally, BF3 was engineered into the electrolyte microenvironment, and it could form adducts with N2, serving as a dynamic carrier for N2 transport. The electron-rich Lewis acidic sites and the dynamic carriers exerted a ‘pull–pull’ effect on N2, thereby weakening the NN bonds. Through electrochemical performance evaluation, the designed electrocatalytic scheme achieved an NH3 yield of ∼57.15 μg h−1 mg−1 and a Faradaic efficiency of ∼15.14 %. We anticipate that this methodology will provide new insights into the development of electrochemical ammonia synthesis, particularly in relation to multifaceted design.

UV-enhanced O2 sensing using β-Ga2O3 nanowires at room temperature

Oxygen sensors based on β-Ga2O3 nanowires were prepared by a chemical vapor deposition method and investigated in detail. β-Ga2O3 nanowires grew on sapphire substrate at 1100 °C with Au as a catalyst. The polycrystalline structure was confirmed according to the X-ray diffraction (XRD) patterns. Scanning electron microscope (SEM) images revealed the average diameter of the nanowires was 150 nm. The ratio of Ga to O was 0.765 according to energy dispersive spectroscopy (EDS) results. Photoluminescence emissions at 445 and 484 nm originated from oxygen vacancies and gallium-oxygen vacancy pairs. Both EDS results and photoluminescence revealed intrinsic oxygen vacancies in β-Ga2O3 nanowires. We coated the β-Ga2O3 nanowires on an interdigitated electrode to fabricated an oxygen sensor. Under ultraviolet light irradiation, at room temperature, the sensor’s response rise time and recovery time were 1034 s and 1283 s to 600 ppm oxygen, those were 1290 s and 1709 s to 1200 ppm oxygen. The mechanism of oxygen sensing was discussed.

Microstructure and properties of Cu-doped β-Ga2O3 rod prepared with liquid metallic gallium

One-dimensional β-Ga2O3 is expected for potential applications in electronics, sensors, and optoelectronics. Gallium hydroxide (GaO(OH)) with different Cu doping was prepared via the hydrothermal method using liquid metallic gallium and copper chloride dihydrate (CuCl2·2H2O) as the starting materials. The material was then transformed to β-Ga2O3 after calcination at 800 °C. SEM images reveal that the obtained powders are well dispersed and have a uniform rod morphology with a length of 13–14 μm and a width of approximately 500 nm. The addition of Cu ion significantly improves the surface morphology of the rod and effectively inhibits the generation of intrinsic oxygen vacancies. And the relative Fermi energy level of Cu-doped β-Ga2O3 undergoes a notable shift from 2.81 eV to 1.25 eV, suggesting the formation of p-type conductivity. Meanwhile, the PL spectra of the Cu-doped samples exhibit emission peaks in the red wavelength range, which is expected for new applications.

Shape-controlled growth of beta-gallium oxide nanowires and experimental investigation on the origination of electrons

Diameter-controlled growth of monoclinic gallium oxide nanowires was performed by chemical vapor deposition technique. Prior to growth, a thin layer of Au films was fabricated, SEM images indicated that Au could converge nanoparticles to govern the growth of β-Ga2O3 nanowires. The SEM images revealed both diameter and length of β-Ga2O3 nanowires strongly depended on the growth temperature. Nanowires grown at 1100 °C temperature have the minimum diameters and uniform lengths, compared with those grown at 900 °C and 1000 °C. The reasons are that a combination and a competition of vapor-liquid-solid (VLS) and vapor-solid (VS) mechanism occur in the growth process. High temperature would provide enough energy to make Ga and O atoms grow along one-dimensional axial orientation following the VLS mechanism. However, low temperature confines atoms at the nanowires interface and enhance sidewalls coalescence following the VS mechanism. X-ray diffraction (XRD) patterns and refinement indicated that the grown samples were of high crystallinity and had intrinsic oxygen vacancies. Photoluminescence spectra were examined and then followed by Gaussian fitting. Through analysis, the emission peaks were considered to originate from intrinsic oxygen vacancies and Ga-O vacancy pairs, consisting with the XRD refinement results. β-Ga2O3 nanowires was coated on the interdigitated electrode, the response to the ultraviolet light and oxygen was studied.

Tunable Ferroionic Properties in CeO2/BaTiO3 Heterostructures.

Ferroionic materials combine ferroelectric properties and spontaneous polarization with ionic phenomena of fast charge recombination and electrodic functionalities. In this paper, we propose the concept of tunable polarization in CeO2-δ (ceria) thin (5 nm) films induced by built-in remnant polarization of a BaTiO3 (BTO) ferroelectric thin film interface, which is buried under the ceria layer. Upward and downward fixed polarizations at the BTO thin film (10 nm) are achieved by the lattice termination engineering of the SrO or TiO2 terminated Nb:SrTiO3 (NSTO or STN) substrate. We find that the ceria layer punctually replicates the polarization of the BTO interface via a dynamic reconfiguration of its intrinsic defects, i.e., oxygen vacancies and small polarons. Tunable oxidative or reducing properties (redox) also arise at the surface from the built-in polarization. Opposite polarities at the ceria termination tune the chemo-physical dynamics toward water molecule adsorbates. The inversion of the surface potential leads to a modulation of the water adsorption-desorption equilibrium and water ionization (splitting) redox overpotentials within ±400 mV at room temperature, depending on the ceria termination's charges. Such tunability opens up the perspectives of using ferroionics for wireless electrochemically enhanced catalysis.

Rationalizing Defective Biomimetic Ceria: In Vitro Demonstration of a Potential “Trojan Horse” Nanozyme Based‐Platform Leveraging Photo‐Redox Activities for Minimally Invasive Therapy

AbstractSemiconductor nanostructures with surface defect‐mediated chemistry have garnered pronounced interest due to their exceptional photo‐induced intracellular bio‐catalytic (enzyme‐mimicking) responses. However, designing defective nanozymes with pH‐responsive multi‐bio‐catalytic functions without any dopants is challenging. Herein, oxygen‐deficient “trojan horse‐like” folate‐functionalized, L‐arginine‐coated ceria (FA‐L‐arg‐CeO2) nanozymes with synergistic multi‐enzyme‐mimicking and anti‐cancer potential are introduced. Intrinsic surface oxygen vacancies (VO●) are strategically created in the nanozymes under kinetically favorable synthesis conditions. Increased surface VO● promotes band structure reconstruction and amplified photochemical‐response efficacy under single laser irradiation (808 nm), outperforming the defect‐free commercial nano‐CeO2 in rapid anti‐tumorigenic activities. Through folate receptor‐mediated endocytosis, these biostable nanozymes localized in MDA‐MB‐231 cells (84% in 48 h) and demonstrated NIR‐accelerated enzymatic functions depending on the pH of the biological milieu. The reduced band gap energy facilitated effective electron‐hole separation, up‐regulating in vitro photo‐redox reactions that impart exceptional therapeutic potential and inhibit 62% cell metastasis within only 12 h. By perturbing intratumoural redox homeostasis, VO●‐rich FA‐L‐arg‐CeO2 nanozymes unanimously killed 86% of MDA‐MB‐231 cancer cells while preferentially shielding benign L929 cells. Transcending beyond conventional drug‐loaded or dopant‐incorporated‐CeO2 nanoplatforms, these defective multi‐modal nanozymes unravel a new avenue for developing smart, low‐cost, bio‐active agents with enhanced efficacy and bio‐safety.

Exploring the Impact of Oxygen Vacancies in Co/Pr-CeO2 Catalysts on H2 Production via the Water-Gas Shift Reaction.

In this study, we utilized various Pr-doped CeO2 catalysts (Pr=5, 10, 20, and 30 wt.%) as a support medium for the dispersion of cobalt (Co) nanoparticles, aiming to investigate the impact of oxygen vacancies on the water-gas shift (WGS) reaction. Different characterization techniques were employed to understand the insights into the structure-activity relationship governing the performance of Pr doped ceria supported Co catalysts towards WGS reaction. Our findings reveal that Co/Pr-CeO2 catalysts at optimum Pr loading (10 wt.%) exhibit a superior CO conversion (88 %) facilitated by the presence of more oxygen vacancies induced by Pr doping into the CeO2 lattice, as opposed to the performance of the pure Co/CeO2 catalytic system. It was also found that the highest activity was obtained at increased intrinsic oxygen vacancies and strong synergy between Co and Pr/CeO2 support, fostering more favorable CO activation at the interfacial sites, thus accounting for the observed enhanced activity.

Oxygen Vacancy Enabled Electronic Structure Engineering of Pt-WO3 Nanosheets toward Highly Efficient BTEX Sensing.

A Pt nanoparticle-immobilized WO3 material is a promising candidate for catalytic reactions, and the surface and electronic structure can strongly affect the performance. However, the effect of the intrinsic oxygen vacancy of WO3 on the d-band structure of Pt and the synergistic effect of Pt and the WO3 matrix on reaction performance are still ambiguous, which greatly hinders the design of advanced materials. Herein, Pt-decorated WO3 nanosheets with different electronic metal-support interactions are successfully prepared by finely tuning the oxygen vacancy structure of WO3 nanosheets. Notably, Pt-modified WO3 nanosheets annealed at 400 °C exhibit excellent benzene series (BTEX) sensing performance (S = 377.33, 365.21, 348.45, and 319.23 for 50 ppm ethylbenzene, benzene, toluene, and xylene, respectively, at 140 °C), fast response and recovery dynamics (10/7 s), excellent reliability (σ = 0.14), and sensing stability (φ = 0.08%). Detailed structural characterization and DFT results reveal that interfacial Ptδ+-Ov-W5+ sites are recognized as the active sites, and the oxygen vacancies of the WO3 matrix can significantly affect the d-band structure of Pt nanoparticles. Notably, Pt/WO3-400 with improved surface oxygen mobility and medium electronic metal-support interaction facilitates the activation and desorption of BTEX, which contributes to the highly efficient BTEX sensing performance. Our work provides a new insight for the design of high-performance surface reaction materials for advanced applications.

Direct Catalytic Conversion of Carbon Dioxide to Liquid Hydrocarbons over Cobalt Catalyst Supported on Lanthanum(III) Ion‐Doped Cerium(IV) Oxide

AbstractDirect CO2 conversion to liquid hydrocarbons (HCs) in a single process was achieved using cobalt (Co) catalysts supported on lanthanum ion (La3+)‐doped cerium oxide (CeO2) under a gas stream of H2/CO2/N2=3/1/1. The yield of liquid HCs was the highest for 30 mol% of La3+‐doped CeO2, which was because extrinsic oxygen vacancy formed by doping La3+ could act as an effective reaction site for reverse water gas shift reaction. However, the excess La3+ addition afforded surface covering lanthanum carbonates, resulting in depression of the catalytic performance. On the other hand, bare CeO2 lead to an increase in the selectivity of undesirable methane, which arose from reduction of CO2 to CO proceeding by intrinsic oxygen vacancy generated by only Ce3+, and weaker CO2 capture ability of intrinsic oxygen vacancy than extrinsic one, resulting in the proceeding of Sabatier reaction on Co catalyst. The rational design of reaction sites presented in this study will contribute to sustainability.

Catalytic properties of trivalent rare-earth oxides with intrinsic surface oxygen vacancy

Oxygen vacancy (Ov) is an anionic defect widely existed in metal oxide lattice, as exemplified by CeO2, TiO2, and ZnO. As Ov can modify the band structure of solid, it improves the physicochemical properties such as the semiconducting performance and catalytic behaviours. We report here a new type of Ov as an intrinsic part of a perfect crystalline surface. Such non-defect Ov stems from the irregular hexagonal sawtooth-shaped structure in the (111) plane of trivalent rare earth oxides (RE2O3). The materials with such intrinsic Ov structure exhibit excellent performance in ammonia decomposition reaction with surface Ru active sites. Extremely high H2 formation rate has been achieved at ~1 wt% of Ru loading over Sm2O3, Y2O3 and Gd2O3 surface, which is 1.5–20 times higher than reported values in the literature. The discovery of intrinsic Ov suggests great potentials of applying RE oxides in heterogeneous catalysis and surface chemistry.

High Proton Conduction in the Octahedral Layers of Fully Hydrated Hexagonal Perovskite-Related Oxides.

Proton conductors have potential applications such as fuel cells, electrolysis cells, and sensors. These applications require new materials with high proton conductivity and high chemical stability at intermediate temperatures. Herein we report a series of new hexagonal perovskite-related oxides, Ba5R2Al2SnO13 (R = Gd, Dy, Ho, Y, Er, Tm, and Yb). Ba5Er2Al2SnO13 exhibited a high proton conductivity without chemical doping (e.g., 0.01 S cm-1 at 303 °C), which is attributed to its high proton concentration and diffusion coefficient. The high diffusion coefficient of Ba5Er2Al2SnO13 can be attributed to the fast proton migration in the octahedral layers. The high proton concentration is attributed to full hydration in hydrated Ba5Er2Al2SnO13 and the large amount of intrinsic oxygen vacancies in the dry sample, as evidenced by both neutron diffraction and thermogravimetric analysis. Ba5Er2Al2SnO13 was found to exhibit high chemical stability under wet atmospheres of O2, air, H2, and CO2. High proton conductivity and high chemical stability indicate that Ba5Er2Al2SnO13 is a superior proton conductor. Ba5R2Al2SnO13 (R = Gd, Dy, Ho, Y, Tm, and Yb) exhibited high electrical conductivity in wet N2, suggesting that these materials also exhibit high proton conductivity. These findings will open new avenues for proton conductors. The high proton conductivity via full hydration and fast proton migration in octahedral layers in highly oxygen-deficient hexagonal perovskite-related materials would be an effective strategy for developing next-generation proton conductors.

Improved resistive switching behavior of defective fluorite structured Sm2Ce2O7 thin film prepared by RF sputtering

The Al/Sm2Ce2O7/ITO (Al/SCO/ITO) structure resistive random access memory (RRAM) was prepared using RF magnetron sputtering, and its resistive switching (RS) behaviors were systematically investigated. The memory exhibited a high switching cycle of 1031, along with set/reset voltages of −1.55/0.53 V and a Ron/Roff ratio exceeding 102. This high performance can be attributed to the presence of intrinsic oxygen vacancies in the defective fluorite structure, accounting for 34.44 % of the vacancies. This vacancy percentage can be increased to 41.97 % by simultaneously transforming Ce4+ to Ce3+ ions through annealing treatment, thereby releasing additional oxygen vacancies. Despite this increase, there remains a sufficient window (Ron/Roff > 10) to distinguish between the high-resistance state (HRS) and low-resistance state (LRS) of the SCO device. Furthermore, the device, when subjected to post-metal annealing (PMA), exhibits a high endurance of up to 1815 cycles, a set/reset voltages of −2.19/1.31 V, a Ron/Roff ratio of >10, and a retention time of over 104 s at 25 °C and 85 °C. However, it is important to note that PMA-treated device requires a higher forming voltage due to the formation of a thicker AlOx layer. This study highlights the potential of Al/SCO/ITO memory devices for RRAM applications.

Exploring tungsten-oxygen vacancy synergy: Impact on leakage characteristics in Hf0.5Zr0.5O2 ferroelectric thin films

The recent discovery of ferroelectric properties in HfO2 has sparked significant interest in the fields of nonvolatile memory and neuromorphic computing. Yet, as device scaling approaches sub-nanometer dimensions, leakage currents present a formidable challenge. While tungsten (W) electrodes are favored over traditional TiN electrodes for their superior strain and interface engineering capabilities, they are significantly hampered by leakage issues. In this study, we elucidate a positive feedback mechanism attributable to W electrodes that exacerbates oxygen vacancy defects, as evidenced by density functional theory computations. Specifically, intrinsic oxygen vacancies facilitate the diffusion of W, which, in turn, lowers the formation energy of additional oxygen vacancies. This cascade effect introduces extra defect energy levels, thereby compromising the leakage characteristics of the device. We introduce a pre-annealing method to impede W diffusion, diminishing oxygen vacancy concentration by 5%. This reduction significantly curtails leakage currents by an order of magnitude. Our findings provide a foundational understanding for developing effective leakage suppression strategies in ferroelectric devices.

High entropy pyrochlore (La0.3Gd0.3Ca0.4)2(Ti0.2Zr0.2Hf0.2Nb0.2Ta0.2)2O7 ceramic with amorphous-like thermal conductivity for environmental/thermal barrier coating applications

Low thermal conductivity and excellent mechanical strength are essential to pyrochlore A2B2O7 ceramic for environmental/thermal barrier coating applications. To collaboratively tailor the mechanical and thermal properties of A2B2O7 ceramic, a novel high entropy pyrochlore ceramic (La0.3Gd0.3Ca0.4)2(Ti0.2Zr0.2Hf0.2Nb0.2Ta0.2)2O7 with significant atomic radius and mass fluctuation is proposed by simultaneously introducing various elements with different valence states at A and B cation sites. The as-synthesized (La0.3Gd0.3Ca0.4)2(Ti0.2Zr0.2Hf0.2Nb0.2Ta0.2)2O7 exhibits enhanced fracture toughness (1.68 MPa m1/2), amorphous-like low thermal conductivity (1.45 W m–1 K–1 at 900 °C) and matched thermal expansion coefficient (9.0 × 10–6 K–1 at 1200 °C) with Al2O3/Al2O3 CMCs. The extensive misfits in atomic weight, ionic radius among the substitutional cations in combination with the intrinsic oxygen vacancies in the anion sublattice play significant roles in the thermal conductivity reduction of (La0.3Gd0.3Ca0.4)2(Ti0.2Zr0.2Hf0.2Nb0.2Ta0.2)2O7 ceramic. The combination of outstanding mechanical and thermal properties indicates that this type of material has a good application prospect for environmental/thermal barrier coatings.

High-efficiency photocatalyst based on Au nanoparticles loaded on defective ZnO nanorods

Optimizing the semiconductor-metal interaction is the key to developing metal single-atom cocatalysts with 100 % metal atom utilization and unique electronic properties. Metal atom sites are exclusively coordinated with semiconductor, featuring a chemical-bond-driven tunable interaction. Here vacancy defect-rich ZnO nanorods (NRs) are fabricated by a facile hydrothermal approach. Au nanoparticles (NPs) are preferentially anchored on surface zinc vacancy sites of ZnO NRs in an ultra-low concentration (10−4 mol/L) of HAuCL4 solution. The Au/ZnO nanohybrids exhibit an excellent photocatalytic activity toward removal of Rhodamine B and levofloxacin. Combining ferromagnetism and valence-band XPS spectra analysis, it is demonstrated that the strong interaction of surface vacancy defects in ZnO and Au generates a distinct upshift of the valence band edge, resulting from the antibonding interaction between O 2p and Au 5d orbitals which significantly weakens the Au–O bonds. This facilitates the release of the lattice oxygen and thus generates more oxygen vacancies. The remarkable photoactivity of defective Au/ZnO is due to the synergistic interaction between the intrinsic oxygen vacancy and Au. Optimizing the hybridization of transition metal d and O 2p states at the atomic scale can induce more active-sites, improve atomic utilization efficiency and thus provide a new approach for enhancing photoactivity.

Oxygen vacancies modulating performance for Ga2O3 solar-blind photodetectors via low-cost mist chemical vapor deposition

The wide bandgap and excellent chemical and physical properties of gallium oxide (Ga2O3) make it an ideal and natural material for solar-blind photodetectors (SBPDs). However, the development of Ga2O3-based SBPDs in practical applications was hindered by intrinsic oxygen vacancies (VO) in Ga2O3 films, high process requirements, and expensive equipment. Here, VO concentration in the films can be regulated by the introducing of O2 in the carrier gases using the mist chemical vapor deposition (Mist-CVD), which has the benefits of low cost, vacuum-free, and easy procedure. The high-performance Ga2O3 films exhibit a single-crystal tendency and low VO concentration under the Ar (1 L/min) and O2 (0.5 L/min) flow rates at 600 °C. The photodetectors exhibit a large photo-to-dark current ratio of 3.0 × 107, a high specific detectivity of 3.06 ×1011 Jones, and a fast response speed of 0.528/0.158 s at 500 μWcm−2 light intensities at 5 V. The mechanism of VO regulation in Ga2O3 films was demonstrated by adjusting the carrier gas flow rates. We also clarified the effect of VO on the dark current and photocurrents of the devices. The low-cost and straightforward Mist-CVD can provide an effective method to grow high-quality Ga2O3 films, further facilitating their practical application.