RESUMEN

Cerium and cobalt loaded Co-Ce/TiO2 catalyst prepared by impregnation method was investigated for photothermal catalytic toluene oxidation. Based on catalyst characterizations (XPS, EPR and H2-TPR), redox cycle between Co and TiO2 (Co2+ + Ti4+ ↔ Co3+ + Ti3+) results in the formation of Co3+, Ti3+ and oxygen vacancies, which play important roles in toluene catalytic oxidation reaction. The introduction of Ce brings in the dual redox cycles (Co2+ + Ti4+ ↔ Co3+ + Ti3+, Co2+ + Ce4+ ↔ Co3+ + Ce3+), further promoting the elevation of reaction sites amount. Under full spectrum irradiation with light intensity of 580 mW/cm2, Co-Ce/TiO2 catalyst achieved 96% of toluene conversion and 73% of CO2 yield, obviously higher than Co/P25 and Co/TiO2. Co-Ce/TiO2 efficiently maintains 10-hour stability test under water vapor conditions and exhibits better photothermal catalytic performance than counterparts under different wavelengths illumination. Photothermal catalytic reaction displays improved activities compared with thermal catalysis, which is attributed to the promotional effect of light including photocatalysis and light activation of reactive oxygen species.

Asunto(s)

RESUMEN

Magnesium hydride (MgH2) as an ideal hydrogen storage carrier whose hydrogen storage performance can be effectively improved by transition metal-based catalysts. To construct highly active catalysts, much attention has been paid to the regulation of transition metal components while less attention has been paid to non-transition metal components especially oxygen, leading certain limitations. Herein, further improved hydrogen storage performance of MgH2 can be obtained by adjusting oxygen vacancy content in molybdenum trioxide (MoO3) catalyst. Specifically, compared with pure MgH2 (1.1 wt%) and MgH2-10 wt% MoO3 (4.5 wt%), more hydrogen (5.9 wt%) can be released by MgH2-10 wt% MoO3-x (MoO3 with abundant oxygen vacancies) at 300.0 °C within 499.0 s. Besides, superb capacity retention (6.1 wt%, 99.0 %) after 50 isothermal hydrogen ab/desorption cycles can be obtained for MgH2-10 wt% MoO3-x. Through rigorous comparative experiments and theoretical calculations, the excellent catalytic activity of MoO3-x is demonstrated to come from the abundant oxygen vacancies and the active substances (polyvalent Mo and nano-sized MgO) it assists to form during ball milling process. This work verifies the feasibility for further improving the catalytic activity of transition metal-based catalysts by tuning non-transition metal elements and thus provides a new strategy in catalyzed MgH2 system.

RESUMEN

The atomic defect engineering could feasibly decorate the chemical behaviors of reaction intermediates to regulate catalytic performance. Herein, we created oxygen vacancies on the surface of In(OH)3 nanobelts for efficient urea electrosynthesis. When the oxygen vacancies were constructed on the surface of the In(OH)3 nanobelts, the faradaic efficiency for urea reached 80.1%, which is 2.9 times higher than that (20.7%) of the pristine In(OH)3 nanobelts. At -0.8 V versus reversible hydrogen electrode, In(OH)3 nanobelts with abundant oxygen vacancies exhibited partial current density for urea of -18.8 mA cm-2. Such a value represents the highest activity for urea electrosynthesis among recent reports. Density functional theory calculations suggested that the unsaturated In sites adjacent to oxygen defects helped to optimize the adsorbed configurations of key intermediates, promoting both the C-N coupling and the activation of the adsorbed CO2NH2 intermediate. In-situ spectroscopy measurements further validated the promotional effect of the oxygen vacancies on urea electrosynthesis.

RESUMEN

The investigation about the mechanism of crystal plane regulation on the generation of oxygen vacancies remains a challenge. In this paper, BiOBr/FeMoO4 composites were synthesized by precise control of crystal plane growth, and it exhibited the enhanced concentration of oxygen vacancies due to lower formation energy of oxygen vacancies. The composite performs higher photo-Fenton-like ability for degrading oxytetracycline hydrochloride (OTC). Structural analyses and theoretical calculations reveal that crystal plane regulation induces significant changes in oxygen vacancy concentration. The BiOBr/FeMoO4/peroxydisulphate (PDS) /light system, which dominated by the non-radical pathway, degraded 96.8 % ± 1.0 % of OTC within 30 min. The activation mechanism of the system and the degradation pathway of OTC were elucidated. The intermediates in the degradation process of OTC were evaluated using liquid chromatograph-mass spectrometer (LC-MS), toxicity evaluation software tool (T.E.S.T) and soybean germination experiments. This work offers novel insights into the pivotal role of crystal plane directional regulation in the quantitative generation of oxygen vacancies.

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The limited energy density of supercapacitors hampers their widespread application in electronic devices. Metal oxides, employed as electrode materials, suffer from low conductivity and stability, prompting extensive research in recent years to enhance their electrochemical properties. Among these efforts, the construction of core-shell heterostructures and the utilization of oxygen vacancy (VO) engineering have emerged as pivotal strategies for improving material stability and ion diffusion rates. Herein, core-shell composites comprising NiCo2S4 nanospheres and MnO2 nanosheets are grown in situ on carbon cloth (CC), forming nanoflower clusters while introducing VO defects through a chemical reduction method. Density functional theory (DFT) results proves that the existence of VO effectively enhances electronic and structural properties of MnO2, thereby enhancing capacitive properties. The electrochemical test results show that NiCo2S4@MnO2-V3 exhibits excellent 1376 F g-1 mass capacitance and 2.06 F cm-2 area capacitance at 1 A g-1. Moreover, NiCo2S4@MnO2-V3//activated carbon (AC) asymmetric supercapacitor (ASC) can achieve an energy density of 39.7 Wh kg-1 at a power density of 775 W kg-1, and maintains 15.5 Wh kg-1 even at 7749.77 W kg-1. Capacitance retention is 73.1 % after 10,000 cycles at 5 A g-1, and coulombic efficiency reaches 100 %, demonstrating satisfactory cycle stability. In addition, the device's excellent flexibility offers broad application prospects in wearable electronic applications.

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In this work, combining the density functional theory (DFT) calculations and the ab initio molecular dynamics (AIMD) simulations, the water adsorption behavior, including the molecular and the dissociative adsorption on the negatively polarized (0 0 1) surface of ferroelectric PbTiO3 was comprehensively studied. Our theoretical results show that the dissociative adsorption of water is more energetically favorable than the molecular adsorption on the pristine PbTiO3 (0 0 1) surface. It has been also found that introducing surface oxygen vacancies (OV) can enhance the thermodynamic stability of dissociative adsorption of water molecule. The AIMD simulations demonstrate that water molecule can spontaneously dissociate into hydrogen atoms (H) and hydroxyl groups (OH) on the pristine PbTiO3 (0 0 1) surface at room temperature. Moreover, the surface OV can effectively facilitate the dissociative adsorption of water molecules, leading to a high surface coverage of OH group, thus giving rise to a high reactivity for water splitting on defective PbTiO3 (0 0 1) surface with OV. Our results not only comprehensively understand the reason for the photocatalytic water oxidation activity of single domain PbTiO3, but also shed light on the development of high performance ferroelectric photocatalysts for water splitting.

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Electrochemical upcycling of end-of-life polyethylene terephthalate (PET) using renewable electricity offers a route to generate valuable chemicals while processing plastic wastes. However, it remains a huge challenge to design an electrocatalyst with reliable structure-property relationships for PET valorization. Herein, spinel Co3O4 with rich oxygen vacancies for improved activity toward formic acid (FA) production from PET hydrolysate is reported. Experimental investigations combined with theoretical calculations reveal that incorporation of VO into Co3O4 not only promotes the generation of reactive hydroxyl species (OH*) species at adjacent tetrahedral Co2+ (Co2+ Td), but also induces an electronic structure transition from octahedral Co3+ (Co3+ Oh) to octahedral Co2+ (Co2+ Oh), which typically functions as highly-active catalytic sites for ethylene glycol (EG) chemisorption. Moreover, the enlarged Co-O covalency induced by VO facilitates the electron transfer from EG* to OH* via Co2+ Oh-O-Co2+ Td interaction and the following C─C bond cleavage via direct oxidation with a glyoxal intermediate pathway. As a result, the VO-Co3O4 catalyst exhibits a high half-cell activity for EG oxidation, with a Faradaic efficiency (91%) and productivity (1.02 mmol cm-2 h-1) of FA. Lastly, it is demonstrated that hundred gram-scale formate crystals can be produced from the real-world PET bottles via two-electrode electroreforming, with a yield of 82%.

RESUMEN

Photocatalytic fixation of nitrogen to ammonia represents an attractive alternative to the Haber-Bosch process under ambient conditions, and the performance can be enhanced by defect engineering of the photocatalysts, in particular, formation of shallow energy levels due to oxygen vacancies that can significantly facilitate the adsorption and activation of nitrogen. This calls for deliberate size engineering of the photocatalysts. In the present study, pyrochlore Bi2Ti2O7 quantum dots and (bulk-like) nanosheets are prepared hydrothermally by using bismuth nitrate and titanium sulfate as the precursors. Despite a similar oxygen vacancy concentration, the quantum dots exhibit a drastically enhanced photocatalytic performance toward nitrogen fixation, at a rate of 332.03 µmol g-1 h-1, which is 77 times higher than that of the nanosheet counterpart. Spectroscopic and computational studies based on density functional theory calculations show that the shallow levels arising from oxygen vacancies in the Bi2Ti2O7 quantum dots, in conjunction with the moderately constrained quantum confinement effect, facilitate the chemical adsorption and activation of nitrogen.

RESUMEN

A novel Fe-g-C3N4/Bi2MoO6 (FCNB) Z-scheme heterojunction enriched with oxygen vacancy is constructed and employed for the photo-Fenton degradation of tetracycline (TC). The 2% FCNB demonstrates prominent catalytic performance and mineralization efficiency for TC wastewater, showing activity of 8.20 times greater than that of pure photocatalytic technology. Density-functional theory (DFT) calculations and degradation experiments confirm that the formation of Fe-N4 sites induces spin-polarization in the material, and the difference in Fermi energy levels results in the formation of built-in electric field at the contact interface, which facilitates the continuous generation and migration of photogenerated carriers to address the issue of insufficient cycling power of Fe (III)/Fe (II).The reactive radicals persistently target the extremely reactive sites anticipated by the Fukui function, causing the mineralization of TC molecules into "non-toxic" compounds through processes of hydroxylation, demethylation, and deamidation. This work holds significant importance in the domain of eliminating organic pollutants from water.

RESUMEN

Double perovskite (DP) oxides are promising electrode materials for symmetric solid oxide cells (SSOCs) due to their excellent electrochemical activity and stability. B-site cation doping in DP oxides affects the reversibility of phase transformation and exsolution, which plays a crucial role in the catalyst recovery. Yet, few studies have been conducted on this topic. In this study, the Sr2Fe1.5-xCoxMo0.5O6-δ (CSFM, x = 0, 0.1, 0.3, 0.5) DP system demonstrates modulated exsolution and phase transformation reversibility by manipulating the oxygen vacancy concentration. The correlation between Co-doping level and oxygen vacancy concentration is investigated to optimize the exsolution and phase transformation properties. Sr2Fe1.2Co0.3Mo0.5O6-δ (3CSFM) exhibits reversible transformation between DP and Ruddlesden-Popper phases with a high density of exsolved CoFe nanoparticles under redox atmospheres. The quasi-symmetric cell with 3CSFM shows a peak power density of 1.27 W cm-2 at 850 °C in H2 fuel cell mode and a current density of 2.33 A cm-2 at 1.6 V and 800 °C in H2O electrolysis mode. The 3CSFM electrode exhibits robust stability during continuous operation for ≈700 h. These results demonstrate the significant role of B-site doping in designing DP materials capable of dynamic phase transformation in diverse environments.

RESUMEN

Photocatalytic water splitting technology for H2 production represents a promising and sustainable approach to clean energy generation. In this study, a high concentration of oxygen vacancies was introduced into tungsten trioxide (WO3) to create a vacancy-rich layer. This modified WO3 (WO3-x) was then combined with N-doped Zn0.6Cd0.4S through a hydrothermal synthesis, resulting in the formation of a Z-scheme heterojunction composite aimed at enhancing photocatalytic performance. Under visible light, the H2 production activity of the composite reached an impressive 8.52 mmol·g-1 without adding co-catalyst Pt. This corresponds to enhancements of 7.82 and 4.39 times the production yield of pure ZCS and ZCSN, respectively. However, the hydrogen production increased to 21.98 mmol·g-1 when Pt was added as a co-catalyst. Furthermore, an array of characterizations were employed to elucidate the presence of oxygen vacancies and the establishment of the Z-scheme heterojunction. This structural enhancement significantly facilitates the utilization of photo-generated electrons while effectively preventing photo-corrosion of ZCSN, thus improving material stability. Our study provides a new scheme for the incorporation of oxygen-rich vacancy and the construction of Z-scheme heterojunction, demonstrating a synergistic effect that greatly advances photocatalytic performance.

RESUMEN

Given the significant global concern about heavy metal pollution, the development of effective adsorbents to capture pollutants has become an urgent issue. In this work, thiol-functionalized defective Zr-MSA-DMSA was designed by mixing 2,3-dimercaptosuccinic acid and mercaptosuccinic acid, which was applied for the rapid and efficient removal of M(II) (i.e., Pb(II), Hg(II), Cd(II)) from wastewater. Zr-MSA-DMSA exhibited excellent adsorption performance, and the maximum adsorption capacities for Pb(II), Hg(II), and Cd(II) were 715.2 mg g-1, 862.7 mg g-1, and 450.5 mg g-1. In actual wastewater, Zr-DMSA-MSA exhibited up to 97 % M(II) removal efficiency and excellent anti-interference ability. It also maintained good structural stability after five adsorption/regeneration cycles. Thus, the abundant oxygen vacancies and unsaturated adsorption sites on Zr-MSA-DMSA significantly improved the adsorption performance of M(II). Spectral analysis and DFT calculations confirmed that Zr-MSA-DMSA mainly relied on the coordination of sulfur and oxygen atoms, electrostatic attraction and a large number of defective sites to achieve the adsorption of M(II). Fixed bed experiments showed that Zr-MSA-DMSA exhibited a depletion time of 10500 min and a volume of 7.0 L. In summary, Zr-MSA-DMSA holds significant potential for treating heavy metal wastewater and provides potential applications for defect engineering.

RESUMEN

The Ti3C2 quantum dots (QDs)/oxygen-vacancy-rich BiOBr hollow microspheres composite photocatalyst was prepared using solvothermal synthesis and electrostatic self-assembly techniques. Together, Ti3C2QDs and oxygen vacancies (OVs) enhanced photocatalytic activity by broadening light absorption and improving charge transfer and separation processes, resulting in a significant performance boost. Meanwhile, the photocatalytic efficiency of Ti3C2 QDs/BiOBr-OVs is assessed to investigate its capability for oxygen evolution and degradation of tetracycline (TC) and Rhodamine B (RhB) under visible-light conditions. The rate of oxygen production is observed to be 5.1 times higher than that of pure BiOBr-OVs, while the photocatalytic degradation rates for TC and RhB is up to 97.27% and 99.8%, respectively. The synergistic effect between Ti3C2QDs and OVs greatly enhances charge separation, leading to remarkable photocatalytic activity. Furthermore, the hollow microsphere contributes to the enhanced photocatalytic performance by facilitating multiple light scatterings and providing ample surface-active sites. The resultant Ti3C2QDs/BiOBr-OVs composite photocatalyst demonstrates significant potential for environmental applications.

RESUMEN

Photothermal catalytic oxidation is a promising and sustainable method for the degradation of indoor formaldehyde (HCHO). However, the excessively high surface temperature of existing photothermal catalysts during catalysis hinders the effective adsorption and degradation of formaldehyde under static conditions. Catalyst loading and oxygen vacancies (OVs) modulation are commonly employed strategies to reduce the photothermal catalytic temperature and enhance the efficiency of photothermal catalytic oxidation. In this work, a p-n type CuO/TiO2 heterojunction is successfully loaded onto diatomite using a wet precipitation method. Under the irradiation of a 300W xenon lamp, the prepared composite material achieved a 100% removal rate of HCHO within 2 h, with a 98% conversion rate to CO2, surpassing the performance of both individual photocatalysts and thermocatalysts. Additionally, by adjusting conditions such as light irradiation and temperature, we have demonstrated that this material exhibits synergistic photothermal catalytic properties. Based on HRTEM, XPS, Raman, and EPR analyses, the introduction of diatomite as a catalyst support was shown to effectively increase the number of OVs. Experimental results, along with O2-TPD, photoelectrochemical characterization, and radical detection, demonstrate that the presence of OVs enhances the oxidative efficiency of both photocatalysis and thermocatalysis, as well as the UV-Vis-IR photothermal catalytic performance. The ternary composite material generates weak hydroxyl (•OH) and superoxide (•O2-) radical under high-temperature with dark conditions, indicating its catalytic oxidation activity under this condition. The increase in temperature and the expansion of the spectral range both enhance the generation of these radicals. In summary, this work demonstrates that the use of diatomite as a support increases the material's specific surface area and OVs content, thereby enhancing adsorption and photothermal catalysis. It elucidates the enhanced catalytic degradation mechanism of this mineral-based photothermal catalyst.

RESUMEN

Oxygen vacancies (VO) in metal oxide semiconductors play an important role in improving gas-sensing performance of chemiresistive gas sensors. Nonetheless, there is still a lack of clear understanding of the inherent mechanism of the influence of oxygen vacancies on gas sensing due to generally focusing on the concentration of VO. Herein, oxygen vacancies were rationally modulated in WO3 nanoflower structures via an annealing process, resulting in a transformation of VO from neutral (VO0) to a doubly ionized (VO2+) state. Density functional theory (DFT) calculations indicate that VO2+ is significantly more efficient than VO0 for NO2 detection in competition with atmospheric O2. Benefiting from a high concentration of VO2+, the WO3-450 (WO3 annealed at 450 °C) sensor exhibits excellent sensing performance with an ultrahigh sensitivity (3674.1 to 5 ppm NO2), superior selectivity, and long-term stability (one month). Furthermore, the sensor with the wide range of concentration detection not only can detect NO2 gas with parts per million (ppm) but also can detect NO2 with parts per billion (ppb) level concentration, with a high sensibility reaching 2.8 to 25 ppb NO2 and over 100 to 100 ppb NO2. This study elucidates the oxygen vacancy mediated sensing mechanism toward NO2 and provides an effective strategy for the rational design of gas sensors with high sensing performance.

RESUMEN

Perovskite oxides are considered highly promising candidates for oxygen evolution reaction (OER) catalysts due to their low cost and adaptable electronic structure. However, modulating the electronic structure of catalysts without altering their nanomorphology is crucial for understanding the structure-property relationship. In this study, a simple plasma bombardment strategy is developed to optimize the catalytic activity of perovskite oxides. Experimental characterization of plasma-treated LaCo0.9Fe0.1O3 (P-LCFO) reveals abundant oxygen vacancies, which expose numerous active sites. Additionally, X-ray photoelectron spectroscopy and X-ray absorption fine structure analyses indicate a low Co valence state in P-LCFO, likely due to the presence of these oxygen vacancies, which contributes to an optimized electronic structure that enhances OER performance. Consequently, P-LCFO exhibits significantly improved OER catalytic activity, with a low overpotential of 294 mV at a current density of 10 mA cm-2, outperforming commercial RuO2. This work underscores the benefits of plasma engineering for studying structure-property relationships and developing highly active perovskite oxide catalysts for water splitting.

RESUMEN

Activation of the stimulator of interferon genes (STING) pathway by radiotherapy (RT) has a significant effect on eliciting antitumor immune responses. The generation of hydroxyl radical (·OH) storm and the sensitization of STING-relative catalytic reactions could improve radiosensitization-mediated STING activation. Herein, multi-functional radiosensitizer with oxygen vacancies depended mimicking enzyme-like activities was fabricated to produce more dsDNA which benefits intracellular 2', 3'-cyclic GMP-AMP (cGAMP) generation, together with introducing exogenous cGAMP to activate immune response. MnO2@CeOx nanozymes present enhanced superoxide dismutase (SOD)-like and peroxidase (POD)-like activities due to induced oxygen vacancies accelerate the redox cycles from Ce4+ to Ce3+ via intermetallic charge transfer. CeOx shells not only serve as radiosensitizer, but also provide the conjugation site for AMP/GMP to form MnO2@CeOx-GAMP (MCG). Upon X-ray irradiation, MCG with SOD-like activity facilitates the conversion of superoxide anions generated by Ce-sensitization into H2O2 within tumor microenvironment (TME). The downstream POD-like activity catalyzes the elevated H2O2 into a profusion of ·OH for producing more damage DNA fragments. TME-responsive decomposed MCG could supply exogenous cGAMP, meanwhile the releasing Mn2+ improve the sensitivity of cyclic GMP-AMP synthase to dsDNA for producing more cGAMP, resulting in the promotion of STING pathway activation.

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The conversion of woody biomass to H2 through photocatalysis provides a sustainable strategy to generate renewable hydrogen fuel but was limited by the slow decomposition rate of woody biomass. Here, we fabricate ultrasmall TiO2 nanoparticles with tunable concentration of oxygen vacancy defects (VO-TiO2) as highly efficient photocatalysts for photocatalytic conversion of woody biomass to H2. Owing to the positive role of oxygen vacancy in reducing energy barrier for the generation of •OH which was the critical species to oxidize woody biomass, the obtained VO-TiO2 achieves rapid photocatalytic conversion of α-cellulose and poplar wood chip to H2 in the presence of Pt nanoclusters as the cocatalyst. As expected, the highest H2 generation rate in α-cellulose and poplar wood chip system respectively achieve 1146 and 59 µmol h-1 g-1, and an apparent quantum yield of 4.89% at 380 nm was obtained in α-cellulose aqueous solution.

RESUMEN

Photocatalytic nitrogen reduction is a promising green technology for ammonia synthesis under mild conditions. However, the poor charge transfer efficiency and weak N2 adsorption/activation capability severely hamper the ammonia production efficiency. In this work, heteropoly blue (r-PW12) nanoparticles are loaded on the surface of ultrathin bismuth oxychloride nanosheets with oxygen vacancies (BiOCl-OVs) by electrostatic self-assembly method, and a series of xr-PW12/BiOCl-OVs heterojunction composites have been prepared. Acting as a robust support, ultrathin two-dimensional (2D) structure of BiOCl-OVs inhibits the aggregation of r-PW12 nanoparticles, enhancing the interfacial contact between r-PW12 and BiOCl. More importantly, the existence of oxygen vacancies (OVs) provides abundant active sites for efficient N2 adsorption and activation. In combination of the enhanced light absorption and promoted photogenerated carriers separation of xr-PW12/BiOCl-OVs heterojunction, under simulated solar light, the optimal 7r-PW12/BiOCl-OVs exhibits an excellent photocatalytic N2 fixation rate of 33.53 µmol g-1h-1 in pure water, without the need of sacrificial agents and co-catalysts. The reaction dynamics is also monitored by in situ FT-IR spectroscopy, and an associative distal pathway is identified. Our study demonstrates that construction of heteropoly blues-based heterojunction is a promising strategy for developing high-performance N2 reduction photocatalysts. It is anticipated that combining of different defects with heteropoly blues of different structures might provide more possibilities for designing highly efficient photocatalysis systems.

RESUMEN

The electrosynthesis of hydrogen peroxide (H2O2) from O2 or H2O via the two-electron (2e-) oxygen reduction (2e- ORR) or water oxidation (2e- WOR) reaction provides a green and sustainable alternative to the traditional anthraquinone process. Herein, a paired-electrosynthesis tactic is reported for concerted H2O2 production at a high rate by coupling the 2e- ORR and 2e- WOR, in which the bifunctional oxygen-vacancy-enriched Bi2O3 nanorods (Ov-Bi2O3-EO), obtained through electrochemically oxidative reconstruction of Bi-based metal-organic framework (Bi-MOF) nanorod precursor, are used as both efficient anodic and cathodic electrocatalysts, achieving concurrent H2O2 production at both electrodes with high Faradaic efficiencies. Specifically, the coupled 2e- ORR//2e- WOR electrolysis system based on such distinctive oxygen-defect Bi catalyst displays excellent performance for the paired-electrosynthesis of H2O2, delivering a remarkable cell Faradaic efficiency of 154.8% and an ultrahigh H2O2 production rate of 4.3 mmol h-1 cm-2. Experiments combined with theoretical analysis reveal the crucial role of oxygen vacancies in optimizing the adsorption of intermediates associated with the selective two-electron reaction pathways, thereby improving the activity and selectivity of the 2e- reaction processes at both electrodes. This work establishes a new paradigm for developing advanced electrocatalysts and designing novel paired-electrolysis systems for scalable and sustainable H2O2 electrosynthesis.