Low Oxygen Vacancy Concentration Research Articles

Enhanced energy-storage properties in (Bi0.5Na0.5)TiO3 ceramics by doping linear perovskite materials Ca0.85Bi0.1(Sn0.5Ti0.5)O3

For energy storage applications in Bi0.5Na0.5TiO3 (BNT)-based materials, the key challenges are the premature polarization saturation and low breakdown electric field (Eb), which confine the energy storage capacity of BNT and significantly restrict progress in advancing pulsed power capacitors. Hence, the cooperative optimization strategy of band structure and defect engineering was proposed, which successfully obtained a high recoverable energy density of 3.83 J/cm3 and an energy efficiency of 77.9 % in the Bi0.5Na0.5TiO3-0.12Ca0.85Bi0.1(Sn0.5Ti0.5)O3 (BNT-0.12CBST) ceramics. Doping the BNT matrix with CBST has been shown to not only reduce grain size but also enhance relaxor behavior, which collectively improves breakdown strength and delays polarization saturation. Furthermore, the x = 0.12 ceramic also exhibits a commendable discharge power density of 91.9 MW/cm3 and a transient discharge time of 40 ns. The higher resistivity and lower oxygen vacancy concentration are conductive to acquire superior breakdown electric field and energy storage performance. We determine the crystal structure, dielectric and ferroelectric properties of the studied ceramics in a wide range of temperatures and concentrations, and a phase diagram is constructed, which illustrates the complex phases present and their transformation behavior. Our work provides an effective strategy to optimize the energy-storage of dielectric ceramics, and shows great potential for practical applications in pulse power systems.

Improved resistive switching characteristics of solution processed ZrO2/SnO2 bilayer RRAM via oxygen vacancy differential

In this study, a solution-processed bilayer structure ZrO2/SnO2 resistive switching (RS) random access memory (RRAM) is presented for the first time. The precursors of SnO2 and ZrO2 are Tin(Ⅱ) acetylacetonate (Sn(AcAc)2) and zirconium acetylacetonate (Zr(C5H7O2)4), respectively. The top electrode was deposited with Ti using an E-beam evaporator, and the bottom electrode used an indium–tin–oxide glass wafer. We created three devices: SnO2 single-layer, ZrO2 single-layer, and ZrO2/SnO2 bilayer devices, to compare RS characteristics such as the I–V curve and endurance properties. The SnO2 and ZrO2 single-layer devices showed on/off ratios of approximately 2 and 51, respectively, along with endurance switching cycles exceeding 50 and 100 DC cycles. The bilayer device attained stable RS characteristics over 120 DC endurance switching cycles and increased on/off ratio ∼2.97 × 102. Additionally, the ZrO2/SnO2 bilayer bipolar switching mechanism was explained by considering the Gibbs free energy (ΔG o) difference in the ZrO2 and SnO2 layers, where the formation and rupture of conductive filaments were caused by oxygen vacancies. The disparity in the concentration of oxygen vacancies, as indicated by the Gibbs free energy difference between ZrO2 (ΔG o = −1100 kJ mol−1) and SnO2 (ΔG o = −842.91 kJ mol−1) implied that ZrO2 exhibited a higher abundance of oxygen vacancies compared to SnO2, resulting in improved endurance and on/off ratio. X-ray photoelectron spectroscopy analyzed oxygen vacancies in ZrO2 and SnO2 thin films. The resistance switching characteristics were improved due to the bilayer structure, which combines a higher oxygen vacancy concentration in one layer with a lower oxygen vacancy concentration in the switching layer. This configuration reduces the escape of oxygen vacancies to the electrode during RS.

Enhancement of oxygen separation performance through Pr0.6Sr0.4FeO3-δ perovskite by modulation of oxygen vacancies

Perovskite-type oxides are promising for oxygen separation purification as oxygen uptake materials. However, their separation performance is limited by the low concentration of oxygen vacancies. Hence, in this work, the low valence Cu is doped to introduce more oxygen vacancies, and a series of Pr0.6Sr0.4Fe1-xCuxO3-δ (x = 0, 0.05, 0.1, 0.15) oxides have been developed to investigate the effects of the Cu contents on the oxygen separation performance. The introduction of Cu in Pr0.6Sr0.4FeO3-δ effectively regulates the concentration of oxygen vacancies and significantly reduces the average metal–oxygen bond energy, thus promoting oxygen separation performance. Especially, Pr0.6Sr0.4Fe0.9Cu0.1O3-δ exhibited the enhanced oxygen adsorption capability (0.195 mmol·g−1) and average desorption rate (7.8 μmol·g−1·min−1) at 600 °C, which are 1.35 and 1.78 times of the parent Pr0.6Sr0.4FeO3-δ respectively. This work provides a successful strategy for optimizing the oxygen separation performance of perovskite materials.

The ultra-high electric breakdown strength and superior energy storage properties of (Bi0.2Na0.2K0.2La0.2Sr0.2)TiO3 high-entropy ferroelectric thin films

The electric breakdown strength (Eb) is an important factor that determines the practical applications of dielectric materials in electrical energy storage and electronics. However, there is a tradeoff between Eb and the dielectric constant in the dielectrics, and Eb is typically lower than 10 MV/cm. In this work, ferroelectric thin film (Bi0.2Na0.2K0.2La0.2Sr0.2)TiO3 with a dielectric constant of 115 is found to exhibit an ultra-high Eb = 10.99 MV/cm, attributing to the high-entropy effects that could result in dense nanostructures with refined grains, low concentration of oxygen vacancies, low leakage current and small polar nano-regions in the thin film. A recoverable energy storage density of 5.88 J/cm3 with an excellent energy storage efficiency of 93% are obtained for the dielectric capacitor containing the thin-film dielectrics. Remarkably, the dielectric capacitor possesses a theoretical energy storage density of 615 J/cm3 compatible to those of electrochemical supercapacitors. The high-entropy ferroelectric thin films with ultra-high Eb and superior energy storage properties are much promising dielectrics used in next-generation energy storage devices and power electronics.

Relationship between defect and strain in oxygen vacancy-engineered TiO2 towards photocatalytic H2 generation

Photocatalytic H2 generation is an effective approach to convert solar energy into renewable H2 energy and has drawn great attentions. To improve the catalytic activity, lots of attentions have been paid to developing advanced strategies, of which oxygen vacancy engineering is considered as a promising one. However, oxygen vacancy induced coexistence of defect and strain makes understanding the essential mechanism of enhanced photocatalytic performance elusive and challenging. Here, the classic photocatalyst TiO2 is selected as a paradigm to reveal the relationship between the accompanied defect and strain in boosting H2 generation activity. It is found that oxygen vacancy concentration almost shows a volcano-type trend, while strain exhibits a monotonic decrease with increasing the calcination temperature. An optimal photocatalytic H2 yield of 788 μmol g−1 h−1 is achieved over the TiO2 with high oxygen vacancy concentration but slight strain. This value is 2.5 times higher than the counterpart with low oxygen vacancy concentration and large strain, indicating that oxygen vacancy induced defect instead of strain plays the dominate role in enhancing photocatalytic H2 generation, which is further verified by theoretical calculations and experimental carrier dynamics analysis. This work uncovers the relationship between defect and strain in oxygen vacancy-engineered photocatalysts.

Impact of Bottom Electrode in HfO2-Based Rram Devices on Switching Characteristics

Resistive random-access memory (RRAM) devices with hydrogen plasma treated HfO2 have shown low power switching (1) and good conductance quantization with programing pulsed operation (2) that qualify them to be used for in-memory computing. Engineering the distribution of defects or oxygen vacancies near the top and bottom electrodes has a significant impact on reducing the switching power and improving the multi-level cell (MLC) characteristics of the device. A graded distribution with higher concentration of oxygen vacancies closer to the top electrode (TE) due to hydrogen plasma treatment and lower concentration near the bottom electrode (BE) reduces switching energy (power) (1). However, the impact of the bottom electrode is not well understood. In this work we investigated three RRAM stacks as shown in Figure 1 that have the same top electrode metal (50nm PVD TiN/5nm ALD TiN) and dielectric (HfO2 with hydrogen plasma treatment at the mid-point) but with different BE for each stack: TiN (device A (control)), TiN plus Mo with thermal anneal (device B), and TiN plus Mo with plasma nitridation (device C). Choosing a more inert metal as the BE provides a lower oxygen vacancy concentration at the interface between the BE and the dielectric (3) which in turn reduces the switching power as noted with device C (TiN plus Mo with plasma nitridation) which switches at a minimum compliance current (Icc) of 500pA. It is possible that the presence of nitrogen prevents the increase in oxygen vacancy concentration near the BE. On the other hand, a higher concentration of oxygen vacancies at the BE and the dielectric interface leads to a larger magnitude of band bending and increases the height of Schottky barrier. This possibly leads to an increase in the switching power in device A and device B as compared to device C (3-4). Note that device A (TiN) switched at Icc=30µA and device B (TiN plus Mo with thermal anneal) switched at Icc=8µA, which is superior compared to device A in switching power. This suggests that the alloy of TiN with Mo is reducing the oxygen vacancies near the BE. To study the MLC characteristics of the devices, we performed a train of 36 RESET pulses with fixed amplitude Vp= -1V and pulse width starting at 4µs and increasing by 20µs every 3 pulses, while we applied Vr=0.1V and tr=10µs after each pulse to measure the conductance. Figure 2 shows that device B (TiN plus Mo with thermal anneal) has good MLC with no overlap between the states while device A shows unstable MLC behavior due to time constant variation. Figure 3a shows the results of device C for the same RESET pulse train that was applied to devices A and B. Since device C switches at very low current and voltage, the conductance quantization was unstable after 15 pulses due to overstress of the conductive filament. Figure 3b shows the results after selecting the proper pulse set Vp= -0.5V and pulse width starting at tp=100ns and increasing by 100ns every 3 pulses, while we applied Vr=0.05V and tr=100ns after each pulse, resulting in a better conductance quantization compared to the previous setup. Appropriate engineering of the BE and managing of the oxygen vacancy distribution by hydrogen plasma treatment can significantly reduce the switching power.

Highest-Efficiency Flexible Perovskite Solar Module by Interface Engineering for Efficient Charge-Transfer.

The electron-transport layer (ETL) plays an important role in improving the performance of flexible perovskite solar cells (F-PSCs). Herein, a room-temperature-processed SnO2 :OH ETL is demonstrated, that exhibits reduced defect density, in particular lower oxygen vacancy concentration, with better energy band alignment and more wettable surface for quality perovskite deposition. More importantly, an efficient electron-transfer channel is produced between the ETL and the perovskite layer due to the formation of hydrogen bonds at the interface, resulting in enhanced electron extraction from the perovskite. As a result, the efficiency of a large-area (36.50 cm2 ) flexible perovskite solar module based on MAPbI3 is increased to as high as 18.71%; this is thought to be the highest reported PCE value for flexible perovskite solar modules to date. In addition, it exhibits high durability while maintaining over 83% of its initial PCE after flexing test cycles. Further, F-PSCs with SnO2 :OH show remarkably long-term stability, owing to a high quality of the perovskite film and a strong coupling between the SnO2 :OH and perovskite layer caused by hydrogen bonds, which successfully inhibits moisture permeation.

Dielectric properties of BaTiO3 and Ba0.95Ca0.05TiO3 sintered in a reducing atmosphere

The dielectric materials utilized in high-performance barium titanate-based base-metal electrode multilayer ceramic capacitors (BME MLCCs) must satisfy stringent criteria such as high dielectric constant, low dielectric loss, high insulation resistivity, and reliability. In this investigation, the effects of raw materials, BaTiO3 (BT), and Ba0.95Ca0.05TiO3 (BCT) on densification, microstructure, and dielectric behavior were explored by introducing acceptor and rare earth elements. The findings revealed that BCT could attain densification at a lower sintering temperature of 1275 °C than BT. Moreover, BCT samples displayed relatively smaller grain sizes, resulting in a greater number of grain boundaries, which in turn increased the insulation resistivity. BCT had a lower oxygen vacancy concentration, thus resulting in lower leakage currents at high temperatures than BT. Substituting BCT for BT resulted in higher activation energies for conductivity in the core, shell, and grain boundary. This investigation demonstrates that BCT can enhance the dielectric properties, insulation resistance, and reliability of the BME MLCCs.

Structural, electronic and optical properties of BaTiO3-CoFe2O4 nanocomposites for optoelectronic devices

Structural, electronic and optical properties of BaTiO3 (BTO), CoFe2O4 (CFO) and their nanocomposites are presented. The XRD spectra of composites exhibited the superposed peak patterns of individual compounds with a consistent shift from BTO to CFO phase with the increase in CFO proportion. The XPS analysis revealed a lower concentration of Oxygen vacancies in the composite samples as compared to that in pure CFO. This finding is also confirmed by the consistent transformation of Co from +2 state in CFO to +3 state in the composite samples. The UV–Vis spectroscopy revealed that optical absorption of BTO is limited to the UV regime, however, CFO exhibited the absorption in visible and infrared (IR) region. However, after the formation of BTO-CFO composite, the optical absorption was broadened from UV to IR regions. The magnitude of absorption was further enhanced by increasing the CFO content in the composites.

Orthorhombic phase induced ultra-low operation voltage in La-doped BiFeO3 resistive switching devices

In this study, the effect of La doping on the resistive switching properties of BiFeO3 (BFO) is systematically discussed. It was found that La doping can not only inhibit the volatilization of Bi and thus diminish the intrinsic oxygen vacancy of BFO, but also improve the lattice symmetry of BFO for generating orthorhombic phase BFO. To confirm these microstructural changes and their relation to the resistive switching properties of BFO, the phase structures, chemical compositions, microstructures, energy band structures, and interfacial features of BFO with different La-doping concentrations are characterized. The resistances of BFO devices with different La doping concentrations also show significant differences, especially, the 15 at. % La-doping BFO device exhibits ultra-low operation voltage of only −0.15 V and good cycling consistency due to the integration of low oxygen vacancy concentrations and precipitation of the orthorhombic phase. The multiple effects of La doping on the resistive characteristics of BFO discussed in this paper provide a reference for the application of BFO in the field of resistive memories.

Influence of stabilizers on hydrothermal behavior of zirconia coatings by APS

In recent years, the degradation of zirconia in a humid environment has attracted the attention of researching. In this work, Mg0.09Zr0.91O1.91 (MSZ), Y0.09Zr0.91O1.955 (YSZ) and Ce0.09Zr0.91O2 (CSZ) powders were prepared by co-precipitation method, the corresponding zirconia coatings were fabricated by atmospheric plasma spraying (APS). All coating samples were subjected to hydrothermal treatment to investigate their degradation process in moisture. The evolution of phase composition and microstructure were characterized. Results show that the content of monoclinic phase (m) in MSZ, YSZ and CSZ coating samples increased after hydrothermal treatment, rising by 47 % in MSZ coating, by 31 % in YSZ coating and by 8 % in CSZ coating. The degradation of internal structure of coatings was more serious with the prolongation of hydrothermal treatment time. This is because different stabilizers will cause different oxygen vacancy concentration in the zirconia unit cell, which determines the hydrothermal stability of zirconia. Under the tested condition, CSZ has the lower oxygen vacancy concentration (4 %) than MSZ (11 %) and YSZ (7 %), exhibiting better hydrothermal stability.

Enhancing the photoelectrochemical activity of monoclinic BiVO4 by discretizing oxygen vacancies: insights from DFT calculations.

Monoclinic bismuth vanadate (BiVO4) has emerged as an excellent optically active photoanode material due to its unique physical and chemical properties. Experiments reported that the low concentration of oxygen vacancies enhances the photoelectrochemical (PEC) activity of BiVO4, but the high concentration of oxygen vacancies decreases the charge carrier lifetime. Using time-domain density functional theory and molecular dynamics, we have demonstrated that the distribution of oxygen vacancies has strong effects on the static electronic structure and nonadiabatic (NA) coupling of the BiVO4 photoanode. The localized oxygen vacancies create charge recombination centers within the band gap and enhance the NA coupling between the VBM and the CBM, resulting in fast charge and energy losses. By contrast, the discrete oxygen vacancies can eliminate the charge recombination centers and decrease the NA coupling between the VBM and the CBM, enhancing the PEC activity of monoclinic BiVO4. Our study suggests that the PEC performance of a photoanode can be improved by changing the distribution of oxygen vacancies.

Significantly enhanced piezocatalytic activity of BaTiO3by regulating the quenching process

Under the synergetic effect of a low oxygen vacancy concentration and rapid cooling rate, the air-cooled BTO powder achieved a significantly enhanced piezocatalytic activity, with a large degradation rate constantkof 0.077 min−1and a H2evolution rate of 1.43 mmol h−1g−1.

Enhanced Proton Conduction with Low Oxygen Vacancy Concentration and Favorable Hydration for Protonic Ceramic Fuel Cells Cathode

Protonic ceramic fuel cells (PCFCs), as an efficient energy storage and conversion device, have great potential to solve the serious problems of energy shortage and environmental pollution. Improving the proton conductivity of the promising cathode materials is an effective solution to promote the widespread application of PCFCs at low temperatures (450-650 °C). Herein, considering the high oxygen reduction reaction (ORR) activity of BaCoO3-based perovskite oxide and beneficial proton uptake capacity of Zn-doping, we construct BaCo0.4Fe0.4Zn0.1Y0.1O3-δ (BCFZnY) as the PCFCs cathode, and compare it with the classic triple-conducting cathode BaCo0.4Fe0.4Zr0.1Y0.1O3-δ (BCFZrY). Different from the general strategy of increasing the initial oxygen vacancy concentration of cathode materials, this work unveils that enhancing the hydration of perovskite oxide with low oxygen vacancy concentration is a more effective strategy to accelerate the proton diffusion in the electrode. Therefore, the BCFZnY cathode achieved excellent proton conductivities of 8.05 × 10-3 and 6.38 × 10-3 S cm-1 as obtained by hydrogen permeation measurements and peak power densities of 982 and 320 mW cm-2 in a BaZr0.1Ce0.7Y0.1Yb0.1O3-δ-based anode-supported fuel cell at 600 and 450 °C, respectively.

Significantly enhanced hybrid improper ferroelectricity of Ca3Ti2O7 ceramics by the oxygen vacancy engineering

Ca3Ti2O7 materials with hybrid improper ferroelectricity call tremendous interest due to their great potential in designing novel room-temperature single-phase multiferroics with a strong magnetoelectric coupling effect. However, achieving Ca3Ti2O7-based ceramics with superior room-temperature ferroelectricity remains a crucial challenge. Herein, Ca3Ti2O7 ceramics were prepared by a tartaric acid sol–gel method and sintered in air and oxygen atmospheres, respectively. It was found that the long-time high-temperature sintering in air could lead to the formation of CaTiO3/Ca3Ti2O7/CaTiO3 sandwich structure, and oxygen-enriched sintering could effectively avoid the formation of CaTiO3 phase on the surface. The superior hybrid improper ferroelectricity is attained in Ca3Ti2O7 ceramics sintered in oxygen atmosphere with a higher remnant polarization (3.63 μC/cm2) and lower coercive electric field (72.6 kV/cm) obtained by positive-up and negative-down method, which is better than the ceramic sample sintered in air. The significantly better ferroelectricity is benefited from the synergistic effects of its larger distortion of oxygen octahedron, larger grain size, and lower oxygen vacancy concentration. Due to its low leakage current density, Ca3Ti2O7 ceramics sintered in oxygen atmosphere exhibit the remanent polarization as high as 7.40 μC/cm2 under the conditions of 1 Hz and 200 kV/cm obtained by dynamic hysteresis measurement mode. Furthermore, there are obvious stripe ferroelectric domains, which provide direct evidence for the excellent hybrid improper ferroelectricity of Ca3Ti2O7 ceramics. These findings demonstrate that the oxygen vacancy engineering is an effective strategy to improve hybrid improper ferroelectricity of Ca3Ti2O7 materials.

Domain Switching in BaTiO3 Films Induced by an Ultralow Mechanical Force.

Low-energy switching of ferroelectrics has been intensively studied for energy-efficient nanoelectronics. Mechanical force is considered as a low-energy consumption technique for switching the polarization of ferroelectric films due to the flexoelectric effect. Reduced threshold force is always desirable for the considerations of energy saving, easy domain manipulation, and sample surface protection. In this work, the mechanical switching behaviors of BaTiO3/SrRuO3 epitaxial heterostructure grown on Nb:SrTiO3 (001) substrate are reported. Domain switching is found to be induced by an extremely low tip force of 320 nN (estimated pressure ∼0.09 GPa), which is the lowest value ever reported. This low mechanical threshold is attributed to the small compressive strain, the low oxygen vacancy concentration in BaTiO3 film, and the high conductivity of the SrRuO3 electrode. The flexoelectricity under both perpendicular mechanical load (point measurement) and sliding load (scanning measurement) are investigated. The sliding mode shows a much stronger flexoelectric field for its strong trailing field. The mechanical written domains show several advantages in comparison with the electrically written ones: low charge injection, low energy consumption, high density, and improved stability. The ultralow-pressure switching in this work presents opportunities for next-generation low-energy and high-density memory electronics.

Increased Oxygen Vacancies in CeO2 for Improved Electrocatalytic Nitrogen Reduction Performance.

Electrochemical nitrogen fixation is a sustainable and economical strategy to produce ammonia. However, fabricating efficient electrocatalysts for nitrogen fixation is still challenging. Theoretical predictions prove that the oxygen vacancy is able to modulate the electronic state of CeO2 and enhance its electrical conductivity, thus promoting the electrochemical nitrogen reduction reaction (NRR) process. Herein, CeO2 with high oxygen vacancy concentration was prepared via a two-step pyrolysis strategy of Ce metal-organic frameworks (MOFs, denoted H-CeO2). Compared to CeO2 with low oxygen vacancy concentration synthesized via one-step pyrolysis of Ce-MOFs (denoted L-CeO2), H-CeO2 exhibits a large NH3 yield rate (25.64 μg h-1 mgcat-1 at -0.5 V vs reversible hydrogen electrode, RHE) and high faradaic efficiency (FE, 6.3% at -0.4 V vs RHE).

Lower oxygen vacancy concentration in BiPO4 with unexpected higher photocatalytic activity

Defect engineering has been demonstrated to be an appealing strategy to boost the photocatalytic activity of materials. However, can higher defect concentration bring about higher photocatalytic activity? This is an open question. In this work, BiPO4 photocatalysts with controllable oxygen vacancy concentrations were successfully synthesized. The photocatalytic activity of the obtained BiPO4 photocatalysts was determined by the removal of ciprofloxacin and 4-chlorophenol, as well as CO2 photoreduction. The BiPO4 materials with lower oxygen vacancy concentration could display unexpected higher photocatalytic efficiency. Through the investigation of different factors which may affect the photocatalytic performance, such as crystal structure, morphology, specific surface area, defect, and energy band structure, it can be found that the energy band structure difference was responsible for the enhanced photocatalytic activity.

Theoretical insights into the oxygen supply performance of α-Fe2O3 in the chemical-looping reforming of methane

The chemical looping reforming of methane to syngas is of great significance to the sustainable development of energy and environment, where the oxygen carrier (OC) is the core element of this technology. To study the oxygen migration properties of OCs and the matching problem of oxygen migration rate with the surface catalytic reaction rate, we present a theoretical study by taking the abundant and cheap α-Fe2O3 as the model OC. It is found that the migration rate of lattice oxygen and the dissociation of methane will be enhanced as the concentration of surface oxygen vacancy increases. By comparing the oxygen migration rate with the methane dissociation rate, we reveal that the two rates can match well at a low surface oxygen vacancy concentration, which is the key to the selective production of syngas. Lower or higher surface oxygen vacancy concentration will lead to the products towards carbon dioxide or coke.

Improving the Surface Oxygen Vacancy Concentration of Bi2O4 through the Pretreatment of the NaBiO3·2H2O Precursor as a High-Performance Visible Light Photocatalyst.

The oxygen-deficient bismuth oxide, Bi2O4, synthesized by a typical hydrothermal method using commercial NaBiO3·2H2O as a raw material only has a relatively low concentration of surface oxygen vacancies (OVs). How to improve the visible light photocatalytic performance of Bi2O4 via tuning its surface OV concentration is still a huge challenge. In this study, improving the surface OVs of Bi2O4 was successfully realized through the pretreatment of commercial NaBiO3·2H2O, including thermal treatment in air and hydrothermal treatment in 10 M NaOH solution, forming NaBiO3·xH2O intermediate products first, and then hydrothermal preparation of Bi2O4 target products using NaBiO3·xH2O instead of commercial NaBiO3·2H2O as the precursor. The enhanced surface OV content not only narrows the band gap of Bi2O4 and thus extends its optical response range but also captures more photoexcited electrons and thus increases the charge carriers' separation efficiency and prolongs the charge carriers' lifetime of Bi2O4. Among the above-mentioned two pretreatment methods, the effects of the hydrothermal pretreatment are superior to those of the thermal treatment, involving the increase of surface OVs, the optical harvesting capacity, and the charge carriers' separation efficiency. Accordingly, Bi2O4 prepared by the hydrothermal pretreatment route exhibits the optimal visible light catalytic performance toward the removal of methyl orange (MO) and phenol due to its most abundant surface OV concentration, which is 2.59 times and 4.26 times higher than that of Bi2O4 synthesized directly by the commercial NaBiO3·2H2O route, respectively. Holes (h+) and superoxide radicals (•O2-) are identified as the main active species, while singlet oxygen (1O2) and hydroxyl radicals (•OH) are verified as the second and third important active species for organic pollutant removal, respectively. This work has developed a novel strategy to promote the catalytic performance of single Bi2O4 induced by the enhanced surface OV concentration through the pretreatment of the precursor, commercial NaBiO3·2H2O.