Controlled Fabrication of RuOxSey Composites for Enhanced Acidic Oxygen Evolution

doi:10.21203/rs.3.rs-2352607/v1

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Research Article

Controlled Fabrication of RuOxSey Composites for Enhanced Acidic Oxygen Evolution

https://doi.org/10.21203/rs.3.rs-2352607/v1

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published 12 Jan, 2023

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Developing relatively cost-effective and high-performance Ru-based composites as electrocatalysts for acidic oxygen evolution has become the critical step toward emerging renewable energy conversion, in which exploring controllable synthetic strategies and investigating the intrinsic nature by non-metallic interfacial modulation is highly desirable. In this work, a facile tandem process is proposed by ball-milling and thermal annealing for the scalable synthesis of RuO_xSe_y nanocomposites with in-situ formed crystalline RuSe₂ and metallic Ru heterostructures on RuO₂ substrate. The optimized RuO_xSe_y-800 sample has been proved to an excellent OER activity and long-term stability in an acidic electrolyte due to its suitable microscopic morphology and phase composition, along with a relatively smaller Tafel slope of 45.4 mV dec^− 1 compared with commercial RuO₂ and most similar catalysts reported in the literature. The outstanding acidic OER performance can be ascribed to the enhanced electron transfer and more active site exposure by controllable selenization. This work paves a novel way for the design and large-scale production of various non-metallic modified composite catalysts for extensive applications of energy conversion and storage.

Ru-based catalysts

heterostructures

interfacial modulation

high stability

Oxygen evolution reaction (OER), a crucial half-reaction in many energy-conversion and storage technologies, is often combined with several reactions, such as hydrogen evolution reaction (HER), electron oxygen reduction reaction (ORR), and two-electron hydrogen peroxide (H₂O₂) generation in electrochemical hydrolysis to construct next-generation energy devices and systems [1–5]. Nevertheless, the complex process and sluggish kinetics of OER remain enormous limitations to the efficiency of the overall electrochemical system [6, 7]. Therefore, the development of OER catalysts with low cost, high activity, and long-term stability is of essential scientific and practical significance. Noble metal iridium (Ir) and ruthenium (Ru) based materials are generally considered desired candidates for OER electrocatalysts according to the volcano map of oxygen intermediate binding energy [8, 9]. Particularly, Ru-based materials are considered to be an ideal alternative under acidic conditions due to their lower overpotential as well as their wide availability and cost-effectiveness [10–12]. Nevertheless, the catalytic activity and durability of the reported Ru-based oxides still cannot meet the expectations for practical applications. Therefore, the development of efficient modification strategies to achieve precise regulation and scalable preparation of optimized Ru-based catalysts for acidic OER is of great scientific significance and application value.

It has been broadly reported that the rational introduction of non-metallic elements (e.g., sulfur, phosphorus, boron, selenium, etc.) at the surface or lattice interstices is an effective strategy to significantly enhance the intrinsic electrochemical activity by surface modification, electronic structure modulation or the formation of intermetallic compounds [13–17]. In addition, synergistic interactions between various components can facilitate the tuning of the catalytic active sites and electron transfer processes, thereby accelerating the reaction kinetics [18–22]. For example, Zhang et al. demonstrated a CoFe₂Se₄/NiCo₂Se₄ hybrid nanotube (CFSe/NCSe HNT) catalyst exhibiting excellent OER performance in alkaline environments due to the synergistic interaction at the heterogeneous interface [22]. However, there remains an urgent need to introduce non-metallic elements into Ru-based oxide materials in a controllable and efficient way to achieve their scalable synthesis and enhancement of activity and stability for acidic OER. In the case of selenium (Se) element doping, the reported synthetic approaches are usually performed by wet chemical synthesis or epitaxial selenization, falling short of the precise regulation and scalable preparation due to requirements of complex reaction steps, limited mass transfer, and low production efficiency [23–27]. Therefore, it is necessary to develop a feasible and effective strategy for the preparation of selenium-modified Ru-based composite catalysts with optimized performance for acidic OER.

Herein, we present the fabrication of a RuO_xSe_y composite with heterostructures consisting of crystalline RuSe₂ and metallic Ru on RuO₂ substrate synthesized via a facile two-step mechanical selenization and thermal procedure. The composite synthesized at 800°C in an inert atmosphere was experimentally validated to possess an optimized phase composition and coordination environment. The RuO_xSe_y-800 sample exhibits excellent OER intrinsic activity, charge transfer kinetics, and long-term stability under a chronopotentiometry (CP) test for 18 h. Extremely low overpotentials of 211 and 285 mV are required to achieve 10 and 100 mA cm^− 2 in a 0.5 M H₂SO₄ electrolyte, along with a relatively smaller Tafel slope of 45.4 mV dec^− 1 and more exposure of active sites. This strategy paves a novel route the for design and preparation of high-efficient composite electrocatalyst derived from non-metallic interfacial modulation, which promotes the practical application of such catalysts in the field of energy conversion and storage.

Materials

Selenium powder (Se, 99.9%) was purchased from Macklin Company. Ruthenium (IV) oxide (RuO₂, metal-based, 99.9%), absolute ethanol (C₂H₅OH, 99.8%), and Nafion 117 solution (5 wt.%) were purchased from Aladdin Company. All chemicals were used as received without further processing and purification.

Preparation of RuO_xSe_y composites

The RuO_xSe_y composites were synthesized by a ball milling-heat treatment step. 250 mg of Se powder and 50 mg of RuO₂ were mixed in anhydrous ethanol (20 mL). The mixture was then added to a ball mill capsule with zirconium oxide interior and ball milled at 1700 rpm for about 15 min using a high-energy vibratory ball mill, and the powder mixture was obtained by washing by filtration and drying under vacuum. Finally, the above mixture was placed in a porcelain boat and heat treated in a tube furnace at different temperatures (700°C, 750°C, 800°C, 850°C, and 900°C) for 2 h with a heating rate of 2°C min^− 1 to obtain RuO_xSe_y composites of different components.

Material characterizations

XRD spectra were recorded by a D/MAX 2500 diffractometer (Rigaku, Japan) with Cu Kα-ray incidence. TEM and HRTEM images were obtained by testing on a JEM-2100F instrument with an acceleration voltage of 200 kV and scanning transmission electron microscopy (FE-SEM, S-4800, Japan) equipped with EDS and elemental mapping. XPS was acquired by a Thermo Scientific ESCALAB 250Xi with an excitation source of Al Kα (1487.6 eV) line, C 1s peak (284.8 eV) was used as the calibration source.

Electrochemical measurements

Electrochemical tests were performed on a CHI 760 workstation in a 0.5 M H₂SO₄ electrolyte using a typical three-electrode system. A carbon paper-based catalyst electrode, a carbon rod, and an Ag/AgCl electrode were used as the working, counter, and reference electrodes, respectively. The loading mass of all catalysts on the working electrode in this work was 0.5 mg cm^− 2. The catalyst ink was prepared from each sample or ruthenium dioxide (5 mg) in a solution consisting of 800 ul water, 100 ul ethanol, and 100 ul Nafion117. All measured potentials were calibrated to the reversible hydrogen electrode (RHE) using the following equation:

E _RHE = E_Ag/AgCl + 0.197 + 0.059 × pH - iR

LSV measurements were performed at a scan rate of 5 mV s^− 1, and all polarization curves were iR-corrected to 95%. EIS measurements were performed at 1.5 V (vs. RHE) with a frequency range of 10⁵ to 0.1 Hz. stability performance was further evaluated by ADT using CV cycling between 1.05 and 1.55 V (vs. RHE) at a scan rate of 100 mV s^− 1 and at an initial potential of 1.442 V (vs. RHE) was evaluated by CP..

Electrical properties characterization

A CHI 660E computer-controlled electrochemical workstation (CH Instrument, China) was employed to measure the cyclic voltammetry (CV) and linear sweep voltammetry (LSV) of the AgPH. A PGSTAT101 computer-controlled electrochemical workstation (Autolab, Switzerland) was used to measure the electrochemical impedance spectroscopy (EIS) of the AgPH.

Fabrication and Morphologies

Figure 1 illustrates a facile synthesis process of RuO_xSe_y samples consisting of wet ball-milling and thermal treatment for selenization. The pristine RuO₂ and selenium powder were uniformly mixed by mechanical effects and then annealed in an inert atmosphere. The selenium powder was molten with a controlled heating process to further achieve modulated phase composition and microstructures by elemental doping and interfacial engineering. The effect of selenization temperatures from 700 to 900°C on chemical composition and electro-catalytic performance was systematically investigated, and the optimal annealing temperature was 800°C (denoted as RuO_xSe_y-800). The morphology of the RuO_xSe_y-800 sample was displayed by SEM images in Fig. 2a, showing a smaller size of blocky aggregates compared to pristine RuO₂ substrate, which is attributed to the highly dispersed states by mechanical ball-milling. Figures S1 presented the SEM images of the original RuO₂ and samples synthesized at other temperatures (denoted as RuO_xSe_y-T, where T is the selenization temperature). All ball-milled samples exhibited more dispersed morphological features relative to the RuO₂ substrate, and there is a tendency for agglomeration between the blocks with the increase in annealing temperatures. As shown in Fig. 2b, the well-defined phase boundaries and contrast distinctions observed in the HRTEM image of RuO_xSe_y-800 further demonstrate the optimized multiple phase composition by thermal interfacial engineering. To further determine the specific phase composition, Fig. 2c displayed a well-resolved interface with distinct characteristic spacings of 3.17 Å ascribed to the (110) lattice plane of the RuO₂ phase, 2.05 Å attributed to the (101) lattice plane of the Ru phase and 2.97 Å corresponded to the (200) lattice plane of the RuSe₂ phase, respectively [28–30]. Moreover, the SAED pattern of RuO_xSe_y-800 (Fig. 2d) shows discrete spots indexed to the (101) and (310) planes for the RuO₂ phase, (101) plane for the metallic Ru phase, and (311) plane for the RuSe₂ phase, revealing the formation of heterogeneous phase composition on RuO₂ substrate. The uniform distribution of Ru, O, and Se elements of the composite was also certified by the EDS elemental mapping images of the RuO_xSe_y-800 sample (Fig. 2e-h), corroborating the desired materials formation by design.

Composition and Structural Characterization

The phase compositions and crystal structures of as-prepared RuO_xSe_y samples were determined by powder XRD. As shown in Fig. 3a, only weak diffraction peaks ascribed to the RuSe₂ phase (JCPDS PDF# 80–0670) can be observed on the RuO₂ substrate (JCPDS PDF# 43-1027) for the RuO_xSe_y-700 sample, which is due to the insufficient reduction of Ru species at lower temperatures. In contrast, characteristic peaks indexed to both metallic Ru (JCPDS PDF#06-0663) and RuSe₂ phase can be identified for samples synthesized above 700°C, and the ratio of phases can be derived from the relative intensities of the corresponding diffraction peaks. The proportion of RuSe₂ phase displayed a dynamic regulation procedure of a remarkable decline followed by an increase with rising temperature between 750–900°C. This phenomenon suggests that the state change of Se as the reaction precursor and the temperature-dependent diffusion kinetics have a significant influence on the composition of RuO_xSe_y samples. Particularly, metallic Ru can be produced by redox reactions of Se vapor, and excessive vaporization rates at high temperatures (900°C) can lead to this reaction not proceeding sufficiently. It can be confirmed experimentally that the RuO_xSe_y-800 sample exhibits an optimized phase composition as a composite of metallic Ru, RuSe_2, and RuO₂ substrate, which is compatible with the above SAED results. XPS measurements were further carried out to analyze the electronic structures and chemical valence states of RuO_xSe_y samples. The XPS survey spectrum in Fig. 3b reveals the existence of Ru, O, and Se elements in RuO_xSe_y-800 by selenization treatment. Since the Ru 3d peaks in the XPS spectra overlap with the C 1s, the information on the valence states of the Ru element was analyzed by Ru 3p orbitals. As shown in Fig. 3c, for RuO₂ samples, the peaks with binding energies at 462.4 eV and 484.7 eV correspond to the typical Ru⁴⁺, and the peak pairs at 465.1 eV and 487.4 eV are labeled as the satellite peaks, indicating the dominant existence of + 4 valence states of Ru species [31]. For RuO_xSe_y-800, the 3p_1/2 and 3p_3/2 peaks located at 484.7 eV and 462.4 eV are assigned to Ru⁴⁺ species, whereas the peaks with binding energies of 484.2 eV and 461.9 eV are attributed to Ru⁰, implying the partial reduction of Ru species and regulation of the interfacial chemical states by controlled thermal treatment [20]. In addition, the Ru 3p_3/2 peak is negatively shifted by about 0.25 eV, indicating enhanced electronic interactions at the catalytic interface. For Se 3d spectrum of RuO_xSe_y-800 presented in Fig. 3d, the peaks at binding energies of 55.1 and 56.0 eV assigned to the RuSe₂ phase further confirm the formation of the RuSe₂ phase [32]. The peak at a binding energy of 59.0 eV corresponds to the Se⁴⁺ species and is attributed to the oxidation of selenium on the surface in air [33, 34]. Figure 3e displays the O 1s XPS spectra of the RuO_xSe_y-800 and RuO₂ samples. For RuO_xSe_y-800, the peak at 529.9 eV corresponds to the lattice oxygen species, the peak at 530.1 eV represents the typical surface hydroxide (OH⁻), the peak located at 531.8 eV is attributed to the oxygen vacancy, and the peak at 532.7 eV represents the adsorbed water [35, 36]. The O 1s XPS peaks of RuO_xSe_y-800 are positively shifted to higher binding energy positions compared to pristine RuO₂, indicating the electrons transfer from O to Ru by the incorporation of Se species. In addition, the relative amounts of oxygen vacancies estimated by the corresponding peak area in RuO_xSe_y-800 were significantly increased, indicating that more oxygen vacancies were generated by Se modification, which is beneficial to improving the OER activity [36–38].

Electrocatalytic performance

To evaluate the OER performance of the RuO_xSe_y catalysts synthesized at different temperatures, the linear sweep voltammetry (LSV) curves of different samples were measured at room temperature with a typical three-electrode system in 0.5 M H₂SO₄. As displayed in Fig. 4a, the OER activity of the RuO_xSe_y composites prepared by thermal treatment ranging from 700–900°C was superior to that of RuO₂, indicating the synergistic effect of heterostructures formed by modification of selenium on the enhancement of acidic OER performance. The RuO_xSe_y-800 catalyst with the optimized composition annealed at 800°C exhibits the highest OER activity, achieving an overpotential of 211 and 285 mV to achieve the current density of 10 and 100 mA cm^− 2, which was much better than those of comparative samples and commercial RuO₂. Figure 4b shows the Tafel curves for each catalyst. the Tafel slope of RuO_xSe_y-800 (45.4 mV dec^− 1) is lower than that of RuO_xSe_y-850 (56.7mV dec^− 1), RuO_xSe_y-900 (72.1mV dec^− 1), RuO_xSe_y-750 (74.3mV dec^− 1), RuO_xSe_y-700 (83.5mV dec^− 1) and RuO₂ (95.6mV dec^− 1), indicating that RuO_xSe_y-800 possesses the fastest reaction kinetics [39, 40]. The Nyquist electrochemical impedance spectroscopy (EIS) was performed to evaluate the kinetic rate of the reaction. the EIS plots were fitted analytically using an equivalent circuit diagram consisting of the solution resistance (R_s), the high-frequency interfacial charge transfer resistance (R_ct1), and the low-frequency resistance (R₂) associated with O₂ mass transfer [41, 42]. As shown in Fig. 4c and Table S1, RuO_xSe_y-800 has the smallest semicircle radius (R₂), indicating the lowest resistance and highest charge transfer rate, which facilitates improved OER kinetics at the interface. To reveal the origin of the high OER activity, the electrochemically active surface area (ECSA) was roughly estimated by corresponding double-layer capacitance (C_dl) values obtained in the non-faradaic range of Cyclic voltammetry (CV) scanning at different scan rates (Figure S2). As shown in Fig. 4d, the C_dl values of RuO_xSe_y-800 composites are higher than that of other catalysts, indicating that the as-synthesized composites expose more catalytic active sites [43, 44]. Stability is a key factor in evaluating the performance of OER electrocatalysts. The stability of RuO_xSe_y-800 and RuO₂ were investigated using an accelerated durability test (ADT) and long-term chrono-potentiometry (CP) curves. Figure 4e shows that there is almost no decay after 1000 CV cycles for the RuO_xSe_y-800 samples compared to the significantly decreased activity of the pristine RuO₂ sample. As shown in Fig. 4f, the RuO_xSe_y-800 exhibits superior stability during 18 h of CP testing. The catalyst increased only 28 mV overpotential in the long-time stability test at a current density of 10 mA cm^− 2. In addition, the substantial chemical stability of RuO_xSe_y-800 was also demonstrated by HRTEM images of the sample tested for 18 h in Figure S3 where well-resolved characteristic spacings ascribed to RuSe₂, metallic Ru, and RuO₂ phase could be identified. The electrocatalytic results indicate that the as-synthesized RuO_xSe_y composite exhibits excellent activity and stability in acidic media, which is also superior to most reported high-performance noble metal catalysts (Table S2 and Figure S4).

In summary, a RuO_xSe_y composite with crystalline RuSe₂ and metallic Ru heterostructures on RuO₂ substrate was successfully synthesized via a facile two-step mechanical selenization and thermal procedure. A series of composites with controllable phase compositions were obtained by regulating the temperatures. The composite synthesized at 800°C in an inert atmosphere was experimentally validated to possess an optimized phase composition and coordination environment. The RuO_xSe_y-800 exhibits superior OER activity with only 211 and 285 mV to achieve 10 and 100 mA cm^− 2, along with a Tafel slope of 45.4 mV dec^− 1, largest C_dl value and long-term stability in a 0.5 M H₂SO₄ electrolyte. The optimized acidic OER performance was attributed to enhanced electron transfer and more active site exposure by controllable selenization. This work provides a new strategy for the development of non-metallic modified composite catalysts for practical applications of renewable energy and electrochemical reactions.

Author contributions

Peng Du, Kai Huang, Ming Lei and Haolin Tang conceived the idea and designed the research. Peng Du and Chaoliang Lin prepared the materials and fabricated the electrocatalysts. Peng Du, Chaoliang Lin and Xian He performed the micromorphology experiments and analysis. Peng Du, Zhichuan Zheng and Xinyu Xie performed the structural characterizations and analysis. Peng Du and Kai Huang performed the electrocatalytic experiments and analysis. All the authors contributed to the writing of the paper.

Funding

This study is supported by the National Natural Science Foundations of China (Grant Nos. 51902027, 61874014, 61874013, 51788104, 61974011 and 61976025), the Basic Science Center Program of the National Natural Science Foundation of China (Grant No. 51788104), National Basic Research of China (Grants Nos. 2016YFE0102200 and 2018YFB0104404), Beijing Natural Science Foundation (Grant No. JQ19005), Fund of State Key Laboratory of Information Photonics and Optical Communications (Beijing University of Posts and Telecommunications, P.R. China), BUPT Excellent Ph.D. Students Foundation (CX2022240), Guangdong Hydrogen Energy Institute of WHUT under Guangdong Key Areas Research and Development Program (No. 2019B090909003), Guangdong Basic and Applied Basic Research Foundation (No. 2020B1515120042) and Foshan Xianhu Laboratory of the Advanced Energy Science and Technology Guangdong Laboratory (No. XHD2020-002).

Compliance with ethical standards

Conflict of interest: The authors declare no conflict of interest.

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Controlled Fabrication of RuOxSey Composites for Enhanced Acidic Oxygen Evolution

Status:

Journal Publication

Version 1

Abstract

Figures

Introduction

Materials And Methods

Materials

Preparation of RuO_xSe_y composites

Material characterizations

Electrochemical measurements

Electrical properties characterization

Results And Discussion

Fabrication and Morphologies

Composition and Structural Characterization

Electrocatalytic performance

Conclusion

Declarations

References

Additional Declarations

Supplementary Files

Status:

Journal Publication

Version 1

Controlled Fabrication of RuOxSey Composites for Enhanced Acidic Oxygen Evolution

Status:

Journal Publication

Version 1

Abstract

Figures

Introduction

Materials And Methods

Materials

Preparation of RuOxSey composites

Material characterizations

Electrochemical measurements

Electrical properties characterization

Results And Discussion

Fabrication and Morphologies

Composition and Structural Characterization

Electrocatalytic performance

Conclusion

Declarations

References

Additional Declarations

Supplementary Files

Status:

Journal Publication

Version 1

Preparation of RuO_xSe_y composites