ACS Catalysis
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2025
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IF 13.1
Yuchen Zhang,Songpei Zhang,Yuxue Yue,Mingyi Xiao,Guangyu Cheng,Yilun Pan,Shitong Liu,Chunfa Li,Jia Zhao,Xiaonian Li
The Deacon process is important and highly desired for chlorine recycling in the chlor-alkali industry. Ru-based catalysts have always attracted much attention in the Deacon reaction; however, they are very easy to deactivate. One of the most advanced methods for adjusting the electrical and geometrical configurations of metal centers is lattice strain engineering, which plays a key role in controlling the interactions between adsorbate molecules and catalytic surfaces. In this study, a catalyst was developed via lattice matching between the active site and the support to enhance d-electron density near the Fermi level and strengthen metal–support interactions. The resulting catalyst achieves sustained chlorine production with a conversion rate of 90% and maintains stability for over 200 h during the Deacon process. This work presents a strategy to inhibit the aggregation of RuO2 and a fresh platform for designing highly stable catalysts.
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CHEMICAL ENGINEERING JOURNAL
·
2021
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IF 13.273
Yajie Qian,Jinjing Huang,Jiabin Chen,Gang Xue,Zilin Zhou,Pin Gao
Peracetic acid (PAA) as an emerging disinfectant has raised extensive concern due to its high oxidation capacity and low byproducts formation potential. In this work, RuO 2 supported multi-walled carbon nanotube (MWCNTs) was synthesized and applied to activate PAA to degrade sulfamethoxazole (SMX). PAA could be effectively activated by RuO 2 /MWCNTs (RM). Increasing RM loadings (0.03–0.3 g/L) or PAA dosages (0.25–1.5 mM) generally enhanced the degradation efficiency, the excellent performance in SMX degradation (100%) was achieved at 1 mM PAA, 0.2 g/L RM and neutral conditions. Electron paramagnetic resonance (EPR) techniques and radical scavenging experiments indicated acetylperoxy radical (CH 3 C(O)OO·) and acetoxyl radical (CH 3 C(O)O·) as the major reactive radicals responsible for SMX degradation. X-ray photoelectron spectroscopy (XPS) analysis indicated that the electron transfer of ≡Ru 3+ /≡Ru 4+ involved in the PAA activation. The effect of water matrices was also investigated, HCO 3 – and natural organic matter (NOM) slightly inhibited SMX degradation, while Cl - had little impact on SMX degradation. For the reusability of RM, the SMX removal was still achieved 90% after three consecutive tests. This work provides the potential application of RM/PAA in destructing emerging pollutants.
研究领域:
环境科学
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化学工程
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
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IF 9.9
Qiaohong Su,Rui Sheng,Qingcui Liu,Juan Ding,Pengyue Wang,Xingchao Wang,Jiulin Wang,Yonggang Wang,Bao Wang,Yudai Huang
The rational construction of amorphous-crystalline heterointerface can effectively improve the activity and stability of hydrogen evolution reaction (HER) and oxygen evolution reaction (OER). Herein, RuO 2 /Co 3 O 4 (RCO) amorphous-crystalline heterointerface is prepared via oxidation method. The optimal RCO-10 exhibits low overpotentials of 57 and 231 mV for HER and OER at 10 mA cm −2 , respectively. Experimental characterization and density functional theory (DFT) results show that the optimized electronic structure and surface reconstruction endow RCO-10 with excellent catalytic activity. DFT results show that electrons transfer from RuO 2 to Co 3 O 4 through the amorphous-crystalline heterointerface, achieving electron redistribution and moving the d-band center upward, which optimizes the adsorption free energy of the hydrogen reaction intermediate. Moreover, the reconstructed Ru/Co(OH) 2 during the HER process has low hydrogen adsorption free energy to enhance HER activity. The reconstructed RuO 2 /CoOOH during the OER process has a low energy barrier for the elementary reaction (O*→*OOH) to enhance OER activity. Furthermore, RCO-10 requires only 1.50 V to drive 10 mA cm −2 and maintains stability over 200 h for overall water splitting. Meanwhile, RCO-10 displays stability for 48 h in alkaline solutions containing 0.5 M NaCl. The amorphous-crystalline heterointerface may bring new breakthroughs in the design of efficient and stable catalysts.
研究领域:
材料科学
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催化化学
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理论计算
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PubMed
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Green Energy & Environment
·
2023
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IF 13.3
Yibo Liu,Xing Hu,Chenxi Liu,Shan Zhu,Kezhu Jiang,Feng Liu,Shijian Zheng
RuO 2 has been considered a potential alternative to commercial IrO 2 for the oxygen evolution reaction (OER) due to its superior intrinsic activity. However, its inherent structure dissolution in acidic environments restricts its commercial applications. In this study, we report a novel Pd-doped ruthenium oxide (Pd–RuO 2 ) nanosheet catalyst that exhibits improved activity and stability through a synergistic effect of Pd modulation of Ru electronic structure and the two-dimensional structure. The catalyst exhibits excellent performance, achieving an overpotential of only 204 mV at a current density of 10 mA cm −2 . Impressively, after undergoing 8000 cycles of cyclic voltammetry testing, the overpotential merely decreased by 5 mV. The PEM electrolyzer with Pd 0.08 Ru 0.92 O 2 as an anode catalyst survived an almost 130 h operation at 200 mA cm −2 . To elucidate the underlying mechanisms responsible for the enhanced stability, we conducted an X-ray photoelectron spectroscopy (XPS) analysis, which reveals that the electron transfer from Pd to Ru effectively circumvents the over-oxidation of Ru, thus playing a crucial role in enhancing the catalyst's stability. Furthermore, density functional theory (DFT) calculations provide compelling evidence that the introduction of Pd into RuO 2 effectively modulates electron correlations and facilitates the electron transfer from Pd to Ru, thereby preventing the over-oxidation of Ru. Additionally, the application of the two-dimensional structure effectively inhibited the aggregation and growth of nanoparticles, further bolstering the structural integrity of the catalyst.
研究领域:
材料科学
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电化学
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Nature Communications
·
2025
·Vol. 16
·期 1
·1-9
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IF 15.7
Zheng Wen-Xing,Cheng Xuan-Xuan,Chen Ping-Ping,Wang Lin-Lin,Duan Ying,Feng Guo-Jin,Wang Xiao-Ran,Li Jing-Jing,Zhang Chao,Yu Zi-You,Lu Tong-Bu
Ruthenium dioxide has attracted extensive attention as a promising catalyst for oxygen evolution reaction in acid. However, the over-oxidation of RuO 2 into soluble H 2 RuO 5 species results in a poor durability, which hinders the practical application of RuO 2 in proton exchange membrane water electrolysis. Here, we report a confinement strategy by enriching a high local concentration of in-situ formed H 2 RuO 5 species, which can effectively suppress the RuO 2 degradation by shifting the redox equilibrium away from the RuO 2 over-oxidation, greatly boosting its durability during acidic oxygen evolution. Therefore, the confined RuO 2 catalyst can continuously operate at 10 mA cm –2 for over 400 h with negligible attenuation, and has a 14.8 times higher stability number than the unconfined RuO 2 catalyst. An electrolyzer cell using the confined RuO 2 catalyst as anode displays a notable durability of 300 h at 500 mA cm –2 and at 60 °C. This work demonstrates a promising design strategy for durable oxygen evolution reaction catalysts in acid via confinement engineering.
研究领域:
材料科学
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电化学
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STAR Protocols
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2023
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IF 0
Yuejiao Li,Lisha Wu,Yajun Ding,Zhong-Shuai Wu
Summary The commercial mass production of bifunctional oxygen catalysts with high activity and stability is critical for constructing high-performance lithium-oxygen (Li-O 2 ) batteries, but remains challenging. Herein, we describe a protocol for the scalable fabrication of a 2D bifunctional electrocatalyst of Pt/RuO 2 /graphene by spatial confinement strategy and elaborately evaluate its oxygen reduction/evolution reactions for advanced Li-O 2 batteries. We then detail the synthesis steps for preparing materials followed by assembly and evaluation of the three-electrode systems and coin-type Li-O 2 batteries. For complete details on the use and execution of this protocol, please refer to Li et al. (2023). 1
研究领域:
材料科学
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电化学
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PubMed
Surfaces and Interfaces
·
2025
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IF 6.3
Tian Tang,Kunlu Chen,Xing Wang,Yanggu Liu,Ziwen Zheng,Xiaoqiang Shen,Liya Li,Xueyan Zheng,Shuai Xiao,Yanrong Chen,Xuesen Du
Under technologically relevant oxygen-rich conditions, the reaction mechanism for CO oxidation over platinum group metals (PGMs) is often complicated by oxide formation. Ru, as a special PGM exhibiting "pressure gap" phenomenon, its optimal active state has been proved to be an ultrathin Ru oxide, rather than pure metal like other PGMs. Therefore, it is plausible to suspect that the sharp rise of CO oxidation rate within narrow temperature range for Ru-based catalysts is not solely controlled by the O 2 activation rate. In this study, we investigated this temperature-dependent sharp rise in the CO oxidation rate through experimental and theoretical calculations. In the rate mutation region, diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) detected a rapid increase in CO 2 production as the adsorbed CO species were annihilated, accompanied by a shift in the reaction orders of CO and O 2 from -0.29 and +0.59 (∼205 °C) to +0.94 and +0.15 (∼215 °C), respectively. The thermodynamic phase diagram indicates that the RuO 2 (110) surface consistently accommodates O* species, but fails to form a stable CO* phase when the temperature exceeds 580 K. Density functional theory (DFT) calculations suggest that initiating the Mars-van Krevelen ( M −vK) mechanism at low temperatures requires overcoming a relatively high activation energy (Ea 1 = 1.28 eV), hence CO prefers the Langmuir-Hinshelwood ( L − H ) mechanism on the Ru/TiO 2 surface. However, as the temperature rises, the M −vK mechanism, once initiated, the activation and reaction of O 2 assisted by oxygen vacancies are thermodynamically(△ H = -2.03 eV) and kinetically (Ea 2 = 0.37 eV) more favorable, respectively. This shift from the L − H to the M −vK mechanism significantly enhances the CO oxidation rate on RuO 2 /TiO 2 catalysts.
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VACUUM
·
2024
·
IF 3.8
Ruilin He,Pan Yang,Maoyuan Zhang,Jingchuan Wang,Yawei Hao,Lijun Yang
Exploring efficient and robust electrocatalysts with low cost for hydrogen evolution reaction (HER) is critical for practical application of electrochemical water splitting. Ru-based platinum group electrocatalysts shows great potential in HER, however, Ru suffer from sluggish kinetics of water dissociation for electrochemical reduction of water to hydrogen in alkaline environments . Here, oxygen atoms are introduced into Ru by simple secondary heat treatment to form Ru–O–C bonds to weak the strength of Ru–H bond. The overpotential of the catalyst is only 19 mV at 10 mA cm −2 and the stability is greatly improved. Theoretical calculations reveal that the Ru–O–C structure formed in RuO 2 facilitates the dissociation of H–OH, which is the rate-determining step in alkaline electrolytes , leading to significant improvement in HER activity.
研究领域:
材料科学
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电化学
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Journal of Energy Chemistry
·
2026
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IF 15.6
Fengyu Wu,Fenyang Tian,Menggang Li,Longyu Qiu,Xue Ren,Lin He,Guanghui Han,Tongbo Zhang,Xinyu Wang,Jie Sheng,Weiwei Yang,Yongsheng Yu
Overcoming the mismatched adsorption energies is critical for efficient alkaline hydrogen electrocatalysis, yet modulating the strong Ru–O covalency without compromising structural integrity remains a key challenge. Herein, we address this by introducing ionic Ru–F bonds into selected regions of RuO 2 via tailored chemical bond engineering for enhanced hydrogen evolution and oxidation reactions (HER/HOR). Using fluorine‑doped amorphous RuO 2 (F‑RuO 2 ) nanosheets as a model catalyst, we find that electrons around fluorine atoms can become highly localized, forming ionic-character Ru–F bonds. This design results in a low HER overpotential of 32 mV at 100 mA cm −2 and delivers a high HOR diffusion-limiting current density of 2.98 mA cm −2 , positioning F-RuO 2 among the best‑performing Ru‑based electrocatalysts yet reported. Moreover, the anion-exchange-membrane water electrolyzer with F-RuO 2 can maintain a cell voltage of 1.60 V at 100 mA cm −2 for over 300 h with negligible degradation. In-situ spectroscopic analysis and density functional theory calculations reveal that the formed Ru–F bonds weaken Ru–O covalency and moderately lower the Ru oxidation states, optimizing hydrogen‑intermediate adsorption toward the ideal range and enhancing both HER and HOR electrocatalysis. This work offers fundamental insights into covalent‑bond modulation in amorphous oxides and establishes a generalizable design paradigm for high-performance electrocatalysts in sustainable energy conversion. The ionic Ru–F bonds reduce the covalency of RuO 2 and optimize the adsorption behaviour of the Ru sites, enabling F‑RuO 2 to exhibit superior reaction kinetics and catalytic activity in both HER and HOR. Download: Download high-res image (166KB) Download: Download full-size image
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CRYSTENGCOMM
·
2025
·
IF 2.6
Yixuan Yuan,Chang Liu,Shanshan Liu,Ruimin Ding,Xi Yin
Proton exchange membrane water electrolysis (PEMWE) powered by renewable electricity is a promising technology for green hydrogen production. Ru-based catalysts are a cost-effective alternative to Ir-based counterparts for the oxygen evolution reaction (OER), yet achieving balanced activity and stability remains challenging. In this study, we optimize the performance of RuO2 by constructing RuO2/Ru–Co3O4 heterogeneous interfaces. Our results indicate that RuO2/Ru–Co3O4 catalyst pyrolyzed at lower temperatures exhibits uniformly small particle sizes with abundant heterointerfaces and strong interfacial electronic interactions. Elevated pyrolysis temperatures enlarge catalyst particle sizes, simultaneously decreasing heterointerfaces and weakening the interfacial interactions. In rotating disk electrode experiments, the mass activity of the RuO2/Ru–Co3O4 catalysts is significantly improved compared to the commercial RuO2. This improvement is attributed to the heterogeneous interfaces, which offer greater utilization of active sites and enhanced charge transfer capabilities. Furthermore, the mass activity of the RuO2/Ru–Co3O4 catalysts decreases with increasing pyrolysis temperatures due to the reduction in heterogeneous interfaces. Additionally, the stability of the RuO2/Ru–Co3O4 catalysts is notably superior to that of commercial RuO2, owing to the interfacial electronic interactions. However, this stability is negatively impacted by higher pyrolysis temperatures as the interfacial electronic interactions weaken. In preliminary membrane electrode assembly tests, the RuO2/Ru–Co3O4 catalyst with low Ru loading shows higher activity than commercial RuO2. Further triple-phase boundary optimization of the catalyst layer is needed. These findings contribute to advanced RuO2-based catalyst design for PEMWE.
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ADVANCED MATERIALS
·
2025
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IF 26.8
Anquan Zhu,Heng Liu,Lulu Qiao,Bin Liu,Kunlun Liu,Chuhao Luan,Kai Liu,Yin Zhou,Dewu Lin,Guoqiang Gan,Jiapei Li,Guo Hong,Wenjun Zhang
The electrochemical nitrate reduction reaction (eNO 3 RR) is widely recognized as a promising strategy for sustainable ammonia production and supporting the nitrogen cycle. However, its advancement is impeded by complex behavior of reaction intermediates and the inevitable reconstruction of precatalysts. To address these challenges, the generation and utilization of active hydrogen (*H) are strategically managed by tailoring the RuO 2 /Co 3 O 4 precatalyst and optimizing the electrolyte composition (OH − and NO 3 − concentration), thereby selectively enhancing ammonia formation. Consequently, the in situ reconstructed RuO 2 /Co(OH) 2 catalyst achieves an impressive ammonia yield of 35.9 ± 0.9 mg h −1 cm −2 and a Faradaic efficiency (FE) of 98.1 ± 2.6% at −0.3 V versus RHE. Furthermore, the catalyst shows significant potential for applications in nitrate-rich wastewater treatment and rechargeable Zn-NO 3 − batteries, maintaining stable operation for over 260 hours at 1 mA cm −2 with only a 6 mV increase in the potential window. Mechanistic studies reveal that electron-rich RuO 2 facilitates *H generation through water dissociation, which subsequently migrates to Co(OH) 2 to hydrogenate nitrogenous intermediates, selectively producing ammonia. This study highlights the importance of designing efficient catalytic systems that address both precatalyst reconstruction and the complexities of reactant and intermediate conversion in electrolytes, which are essential for managing the intricate electron and proton transfer processes involved in eNO 3 RR.
研究领域:
电催化
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环境催化
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能源化学
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材料化学
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可持续化学
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废水处理
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电化学工程
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PubMed
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ACS Nano
·
2025
·
IF 16
Yin Qin,Sihao Deng,Xiao-Ye Zhou,Bin Cao,Zhehan Ying,Zilin Yan,Zheng Zhong,Lunhua He,Kaikai Li,Tong-Yi Zhang
RuO2, the benchmark catalyst for the oxygen evolution reaction (OER), has traditionally been considered Pauli paramagnetic; however, recent findings have demonstrated its antiferromagnetic (AFM) properties, hinting at the opportunity to enhance RuO2’s OER performance by manipulating its magnetic traits. In this study, we successfully induced weak ferromagnetism in commercial RuO2, transitioning it from an AFM state using an electrochemical sodiation method. This process resulted in high activity, achieving an overpotential of 145 mV to reach 10 mA cm–2 and extending the service hours by more than 13 times compared to pristine RuO2 in 0.5 M H2SO4. A combination of experimental and theoretical analyses indicated that the sodiation triggers significant surface compressive stress, leading to lattice distortion and disruption of the pristine structural symmetry of RuO2. Consequently, orbital degeneration ensues, prompting individual spin-up d electrons to jump to the high-spin state. This mechanism drives the conversion from AFM to weak FM behavior for RuO2, ultimately yielding exceptional catalytic activity and stability.
研究领域:
材料科学
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电化学
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催化
·
纳米技术
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固态物理
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表面科学
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危险品化学品经营许可证（带存储）