Enduring and Instant H2O2 Generation via Controlled Coupling Transfer

doi:10.21203/rs.3.rs-1655100/v1

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Enduring and Instant H2O2 Generation via Controlled Coupling Transfer

https://doi.org/10.21203/rs.3.rs-1655100/v1

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Extremely slow kinetics and limited accumulation of H₂O₂ during the oxygen reduction reaction, which derives from the negative effects of diffusion-limited and further catalysis, are the grant challenges seriously hindering the development of green H₂O₂ synthesis. Herein, we first controlled the coupling energy of the proton and electron by periodic-potential-driven catalysis, achieving 56-fold greater H₂O₂ accumulation than that generated by constant-potential catalysis. To modulate proton and electron coupling transfer, we employed optimized dual-electrolytes to achieve a rate of 45900 mmol g_cat⁻¹ h^− 1, and provided strong evidence of molecular-level understanding via comprehensive microenvironment simulation. These results were obtained with a pyrolytic metal/reduced cage crystal (RCC1) catalyst with stable performance reaching 3.6 million pulses, which generated products that can be directly utilized for the complete removal of bacteria in 2 seconds from seawater. Our systemic methodology and in situ application are anticipated to aid in the design of innovative catalysts, provide a deep understanding of pulse and electrolyte effects, and aid in the design of a new effective cell system to achieve industry-level H₂O₂ production.

Pulsed catalysis

Slow Kinetics

Limited Accumulation

Hydrogen peroxide (H₂O₂) as the basic chemical for a variety of industries, is widely used in wastewater treatment¹, bio-disinfection², chemical synthesis³, bleaching⁴, and fuel cell in the energy field ^5-7. Harnessing oxygen as a feedstock is a means of achieving green H₂O₂ synthesis and a promising method to overcome the imbalance of a tight supply and an annual increase in demand of more than 5% ⁸. However, the generation of H₂O₂ via the oxygen reduction reaction (ORR) has been considerably hindered by sluggish kinetics and limited H₂O₂ accumulation ^9-10. To overcome these limitations, extensive research ¹⁰ has focused on increasing catalyst selectivity, adding stabilizers to inhibit the hydrogenation of H₂O_2, and accelerating gas diffusion at the electrode to improve oxygen utilization and overcome the slow reaction rate ^{5, 9, 11-12}. Unfortunately, the abovementioned catalysts suffer from carbon oxidation, demetallation of their active sites and carbon corrosion ¹³; the use of additives results in decreased conductivity and phase separation, and the equipment required for acceleration of gas diffusion suffers from low utilization. We, herein, adjusted the power and solvent to achieve the continuous and instant generation of H₂O₂ over a metal/RCC1-cage catalyst, based on molecular and systemic understanding, to address the poor kinetics and productivity.

Synthesis and analysis of a stable catalyst

To achieve high stability and selectivity for the ORR, dynamic covalent chemistry-based synthesis and template-assisted pyrosis (Figs. S1-2) ¹⁴ were adopted to prepare a catalyst consisting of a cavity cage and a cluster ¹⁵. The cage of CC1 with imine ligands that could absorb, secure and confine a size-controlled and quantity-defined (1/6 atom ratio) metal core within the cavity, as reported by Zhang ¹³ (Figs. S3-6). Even after pyrolysis, the cluster was still uniformly isolated and captured by the cage (Figs. 1a-f and S7-24). The simulated charge distribution and transfer number reveal that the fixed electrons were transferred from the cluster to the pyrolytic cage via the electron penetration effect, as indicated by the positive value of the charge density difference (0.936, 1.554 and 1.759 eV) (Figs. 1g and S25), uncovering reciprocal stabilization. Based on the Sabatier principle ¹⁶, the adsorption force between the catalyst and reactant should be neither strong nor weak; the rate-limiting step in the ORR is the adsorption of oxygen, meaning that adsorption needs to be enhanced. The calculated density indicates a narrowed d-band distribution compared to the uncaged metal core, and the d-band center is closer to the Fermi level (from -4.29 eV for Zn to -2.07 eV for Zn/RCC1, from -3.59 eV for Y and -1.46 eV for Y/RCC1 to -1.03 eV for Y₂O₃/RCC1), implying the enhanced adsorption of adsorbates (Figs. 1h and S26). Locking the cluster in the cage prevents aggregation, compromises reagent adsorption and avoids carbon corrosion and bond contraction, thus guaranteeing reciprocal stability and upregulated activity ¹⁷.

To verify the catalytic properties of the above-described electrocatalyst for the ORR, we optimized the electrode preparation conditions through two improved methods (cerium titration and titanium titration) to precisely assess the synthetic H₂O₂ (Figs. S27-28) ¹⁵. The first-principles calculations suggest that the active site is situated on the outer surface of the catalyst because the main contributor to the overall electron density of states is the outer carbon ¹⁸. Accordingly, the overall reaction, including the steps from O₂ to the intermediates -OOH and -OH and from these intermediates to H₂O₂ or H₂O, respectively, were all calculated based on the outer carbon net (Figs. S29-30). The in situ attenuated total reflection surface-enhanced infrared absorption spectroscopy (ATR-SERIES) performed under various potentials proved the existence of several intermediates in the 2e⁻ ORR. In the spectra, a major band at 1222 cm^-1 corresponded to the stretching mode of -OO- from surface-adsorbed *OOH, and the band at 1390 cm^-1 was attributed to the bending mode of -OOH- from the *HOOH intermediate (Fig. 2a) ¹⁹. While the adsorption barrier for the step of O₂to O₂* is the dominant contributor to the thermodynamic barrier of the ORR from a traditional perspective ⁶, this binding barrier drastically decreased for the caged catalysts (Zn/RCC1, Y/RCC1, Y₂O₃/RCC1) compared to their uncaged analogs (Zn, Y, RCC1), as determined from calculations of the Gibbs free energy difference (ΔG) (Fig. 2b). The barrier of dissociation for HOOH* was found to be larger than that of the adsorption for O₂*for the caged catalysts, showing that the rate-limiting step alters the degradation of H₂O₂ rather than the absorption of O₂. This change in maximal barrier implies that the high selectivity for H₂O₂ synthesis of the caged catalyst is a result of the suppressed degradation of H₂O₂. From the Brønsted–Evans–Polanyi relation ²⁰, the activation energy depends linearly on the heat of the reaction, and the activity of pyrolytic catalysts follows the order Y₂O₃/RCC1, Y/RCC1 and Zn/RCC1, with the 2e⁻ ORR favored over the 4e⁻ ORR from a thermodynamic perspective.

Boosting cumulation through controlled potential

Because of the intrinsic instability of H₂O₂ and the further catalysis, the concentration will reach a maximum or even decrease during constant-potential electrocatalysis (Figs. S30-31). Inspired by the spike-time-dependent plastic transmission of bioelectrical signals, we employed intermittent bias during catalysis to surmount the limited accumulation ¹⁵. The pulsed electrocatalysis increased the maximum concentration of H₂O₂ by 56-fold compared to that achieved at a constant potential (Figs. 2c and S32-33). A molecular dynamics simulation (Fig. 2d) showed that the change in the distance and configuration of H₂O₂ near the catalyst surface was dependent on the applied voltage mean that the coupling of proton and electron are modulated. The distance (from 2.85 to 3.2 Å) and the configuration (from 109.119 to 115.493°) of H₂O₂ showed a linear change near the catalyst surface under a continuous bias, while an applied voltage-dependent tendency was observed under pulsed catalysis for two catalysts. When the bias switched from 0.6 to 0 vs. RHE, the H₂O₂ sensitively separated from the surface of Y/RCC1 from 2.66 to 3.4 Å, clear showing that the applied bias increased the adsorption force for H₂O₂. Briefly, the interval power decreased the adsorption and allowed time for H₂O₂ transport away from the surface of the electrode, hindering further catalysis ²¹.

Reliability and universality of the boosted method

The pursuit of maximum accumulation via pulsed electrocatalysis requires a catalyst with ultrahigh environmental and long-term time stability. Our catalyst maintained its properties for the 2e⁻ ORR when the electrolyte was doped with various common ions (Na⁺, Cl^-, K⁺, SO₄^2-, Ca²⁺, Mg²⁺, HCO₃^2–, PO₄^3– and NO^3–). After 3,600,000 pulse cycles of catalysis, the current remained at 3.4×10^-3 A (Fig. 2e and g). In addition, the CC1 template trapped various metals, including precious metals (Pd), transition metals (Fe, Ni and Zn) and rare earth metals (Y, La and Er). These catalysts increased the concentration of H₂O₂ by tens of times based on pulsed electrocatalysis, with a favorable faradaic efficiency detected by RRDE, revealing the favorable universality and reliability of pulsed catalysis (Fig. 2f).

Dual-electrolytes achieving instant producing

The extremely slow kinetics is still a challenge for the 2e⁻ ORR despite the pulsed electrocatalysis method overcoming the concentration problem. Inspired by the halogen inhibiting the decomposition of H₂O₂^{3, 5}, we employed the optimal concentration of NaCl as an electrolyte to stabilize the formed H₂O₂. This optimal concentration was determined from the relationship between the kinetics and the concentration of electrolytes. With increasing electrolyte concentration, the variation in the preparation rate for H₂O₂ gradually increased to a maximum value (at 1 mol/L NaCl) and then ultimately decreased (Figs. 3a, b and S34-35). Moreover, the electrochemically active specific surface area (ECSA) also followed the same correlation, demonstrating that the reason for these results is the increased number of active sites on the electrode (Figs. S36-37). Additionally, we observed that the rate of accumulation of H₂O₂ increased when rare earth metal/RCC catalysts were applied in a 0.1 mol/L H₂SO₄ electrolyte. Diluted acid increased the rate of the ORR by increasing the electron transfer by protons; however, excessive amounts of acid or alkaline promoted the degradation of H₂O₂ (Figs. S38-41). For this experiment, a library of catalytic curves corresponding to the preparation rate of H₂O₂in H₂SO₄ confirmed that the current is negatively increased during short- and long-term catalysis. The ECSA also increased gradually during catalysis and increased significantly after 100000 cycles of cyclic voltammetry scanning in the fresh electrolyte (Figs. S42-43). These observations revealed that the type and concentration of electrolytes considerably influenced the kinetics of the ORR. Based on the electrolyte-dependent kinetics, we applied dual electrolytes (1 mol/L NaCl as the ORR electrolyte and a saturated solution as the OER electrolyte) via a gas diffusion electrode (GDE) to solve the rate-limiting problem ^{5, 22}. Consequently, the final preparation rate reached 45900 mmol g_cat^-1 h^-1, resulting in a maximum accumulation of 3% H₂O₂ (Figs. 3c and S44). This value exceeds the currently relevant levels, and the kinetics increased fivefold relative to the most efficient 2e⁻ ORR electrolytic devices reported to date (Table S1).

Mechanism of modulated electrolytes

The mechanism of the influence of the electrolyte was strong evidenced by ECSA and simulated by finite element analysis and ab initio molecular dynamics (AIMD). Because the increasing bulk concentration together with increasing excess ions signifies the increasing surface charge density, which caused the increasing electric double layer capacitance (C₂) in Fig. S45a strongly demonstrated by the increased ECSA. And the halogen inhibits the further catalysis of H₂O₂^{3, 5}, therefore, the rate of preparing H₂O₂ increases with the increase of electrolyte concentration. The solubility of oxygen decreases with the increasing concentration of NaCl electrolyte solutions causing the decreased preparation rate of H₂O₂in high concentration electrolyte based on the salting-out effect ²³. Therefore, the optimal concentration (1 mol/L NaCl) was determined, and this stabilization of H₂O₂by ahalogen increased the concentration of H₂O₂ near the electrode surface ^{5, 22}. As revealed by the molecular dynamic simulation (Fig. 3d-i), the electroactive species (-OO*, -OOH* and -HOOH*) were far from the surface of the electrode (broadened distribution), and small variations in the band length and angle were observed for the ORR catalyzed by Y₂O₃/RCC1 compared to those of the ORR catalyzed by Y/RCC1. The pulsed catalysis showed a broadened distribution and less transformation of configuration than that achieved by constant catalysis, along with better performance. The finite element simulation results indicated that the distribution of H₂O₂ near the electrode surface broadened when the electrolyte concentration increased during either constant or pulsed electrocatalysis (Figs. 3m-v and S45-49). Pulsed electrocatalysis resulted in a higher and wider distribution of H₂O₂near the catalyst surface than that achieved by a constant potential in a series of electrolyte concentrations, demonstrating that pulsed catalysis has better performance.

The charge accumulation effect ²⁰ was clearly shown by the non-linear in charge-time curve during catalysis in diluted acid, which increased the production of H₂O₂(Figs. S50-51). A sufficient supply of protons creating a pH gradient increased the cell current until reaching the maximal polarization because the selectivity and ECSA are different in various pH (Fig. S52). Which consistent with proton-coupled electron transfer (PCET) instead of hydrogen atom transfer (HAT) decreasing the transfer barrier because electrons and protons were transferred to one receptor and pH dependent to accumulate the charge ^24-27. Under alkaline and neutral conditions, the ORR was accompanied by increased pH, causing an insufficient proton supply ⁶. Finite element analysis also verified that H₂O₂ had a wider distribution in acidic electrolytes ²⁴ than in alkaline and neutral electrolytes (Figs. 3e-g).

In situ application

Given the strong demand for H₂O₂ in water management, we directly used the prepared H₂O₂ coexisting with -OO-, -OH and -OOH intermediates to degrade the dye rhodamine 6G and eliminate Escherichia coli ^{2, 15, 28-29}. In a control experiment, the presence and absence of ORR were investigated for degradation and sterilization. The removal rate reached 100% for the ORR within 2 hours, while a residual of 2.2 ppm remained even after 10 hours during electrolysis without ORR (Fig. S53). Disinfection was complete in less than two minutes for the ORR in 0.9% NaCl, whereas there was still bacterial residue after 2 hours of disinfection during electrocatalysis in the absence of O₂ reduction (Fig. S54). Thus, this in situ application demonstrated a promising future for water treatment through the pulsed catalysis-prepared highly oxidizing substances during the 2e⁻ ORR.

In conclusion, we, herein, steered dual-electrolytes under modulated microenvironment to control proton and electron transfer for H₂O₂, enabling kinetics of 45900 mmol gcat^-1 h^-1 (5-fold greater than the current maximal rate) cumulating 3% H₂O₂ with molecular-level understanding. The further catalysis and instability nature of H₂O₂ were effectively inhibited by periodic-potential-driven catalysis, achieving 56-fold greater H₂O₂ accumulation than that generated by constant-potential catalysis. The catalyst for ORR was prepared from template pyrolysis. A CC1 template as a versatile platform enabling various metals (noble metal, Pd; transition metal, Zn, Fe and Ni; rare-earth metals, La, Er, and Y) trapped, which could maintain its performance after 100000 CV cycles scanning and 3.6 million pulses catalysis and even diversity ions mixing. The prepared H₂O₂ can be directly utilized for completely and sharply removing pollutants and bacteria in seawater. Our systemic methodology and situ application will provide a better comprehension of pulse, and electrolyte effects and an innovative design for effective ORR cell systems anchoring industry-level performance.

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Any methods, additional references, Nature Research reporting summaries, source data, extended data, supplementary information, acknowledgements, peer review information; details of author contributions and competing no interests; and statements of data and code availability are available at the author or from the supplementary information linked to the ***.

Acknowledgements

This work was financially supported by the Natural Science Foundation of China (21978185, 21938006，21603158), the major research project of Natural Scientific Research Foundation of the Higher Education Institutions in Jiangsu Province (17KJA150010), and the Priority Academic Program Development of Jiangsu Higher Education Institutions (PAPD). I am extremely grateful to Prof. Guangxin Duan from the School of Radiology of Soochow University for providing a place for bacterial culture.

Conflicts of interest

There are no conflicts of interest.

Author contributions statement

Y. Y. Zhao conceived and designed the study, analyzed data and wrote the manuscript. The bacterial culture and sterilization under the guidance of supervisor G. X. Duan. The supervisor J. H. He revised the document together with J. M. Lu supervised the project.

There is NO Competing Interest.

SupplementaryMaterials.docx
Enduring and Instant H2O2 Generation via Controlled Coupling Transfer
TOC.jpg
Herein, we introduced the interval bias application assisted by the self-consistent solvents effect boosted the electron transfer based on a caged platform for oxygen reduction to H₂O₂ preparation to overcome the limited-cumulation and slow kinetics in electrochemical oxygen reduction reaction. Consequently, the final preparation rate can reach 45900 mmol g_cat^-1 h^-1, which fivefold to the most efficient value reported to date, obtaining 56-fold greater H₂O₂ maximum accumulation than that generated by constant-potential catalysis.

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