Russian Journal of Physical Chemistry A
·
2024
·Vol. 98
·期 10
·2219-2232
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IF 0.7
Guiling Wu,Zhao Wenli,Yang Xinyue,Niu Xiaopo,Guo Zhen,Liu Danni,Wang Qingfa
Abstract Producing high-density fuel of alkylated decalins from hydrodeoxygenation (HDO) of naphthalene derivatives is an environmentally friendly but still challenging method. Herein, a bifunctional Ru/HZSM-5 catalyst was fabricated by acid treatment (citric acid, oxalic acid, nitric acid) to effectively synthesize the alkylated decalins via HDO of naphthalene derivative. Acid treatment adjusted the acidic site distribution of Ru/HZSM-5. Nitric acid treatment (NA) resulted in more abundance of weak acidic sites which was beneficial for the dehydration process in HDO, and the lowest ratio of BAS/LAS to promote the hydrogenation of alkylated octalins, the rate-determining step of HDO. NA-treated Ru/HZSM-5 showed the highest HDO activity with the highest selectivity of 1,2-dimethyldecalin (74%). Besides, it also presents good HDO activity of naphthalene derivatives to produce high-density hydrocarbons. Therefore, Ru/HZ5-NA is a promising catalyst for the production of alkylated decalins and other high-value biofuels and chemicals.
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Catalysis Science & Technology
·
2025
·
IF 4.2
Chuqiao Song,Wei Cheng,Xiaojie Wu,Shufang Zhao,Ying Tang,Xin Tang,Yao Xu,Lili Lin,Siyu Yao
The one-pot hydrodeoxygenation of lignin-derived (alkyl)-guaiacols to (alkyl)-cyclohexanols with high selectivity is an attractive process for biomass conversion. However, designing catalysts that preferentially cleave etheric CAr–O(R) bonds over hydrogenating aromatic rings under mild conditions remains a significant challenge. In this study, we explore the structure sensitivity of supported Ru catalysts with varying particle sizes (0.6–7.5 nm) and identify the optimal catalyst for selective hydrodeoxygenation. Using a catalyst with 1.5 nm Ru particles, we achieve a ∼95% yield of cyclohexanol from guaiacol under relatively mild conditions (190 °C, 5 bar H2). In situ DRIFTS analysis reveals that the cleavage of CAr–OCH3 bonds occurs preferentially over aromatic ring hydrogenation on the 1.5 nm Ru particles, minimizing side reactions and enhancing cyclohexanol selectivity.
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Nanoscale
·
2025
·Vol. 17
·期 5
·2820-2829
·
IF 5.1
Yiling Ran,Rong Gan,Qin Zhao,Quanlei Ma,Yijing Liao,Yinwei Li,Yi Wang,Yanwei Wang,Yan Zhang
Engineering the local electronic structure of single atom catalysts (SACs) still remains challenging. In this study, a Ru-NiS2 single atom catalyst with a controlled S coordination environment, where Ru single atoms are implanted on a NiS2 nanoflower consisting of plenty of cross-linked nanosheets, has been developed via a facile atom capture strategy. Using Density Functional Theory (DFT) calculations, it has been revealed that the fine-tuned local S coordination environment can optimize the electronic structure of Ru active sites, and reduce the energy barrier of the rate-determining step for the oxygen evolution reaction (OER), thus boosting the electrocatalytic activity, such as a low overpotential of 269 mV at 10 mA cm−2. This work provides new insights into the rational regulation of the local coordination environment for SACs.
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Science Bulletin
·
2024
·
IF 18.8
Yuanqing He,Chongyang Ma,Shiheng Mo,Chung-Li Dong,Wei Chen,Shuo Chen,Huan Pang,Ren Zhi Ma,Shuangyin Wang,Yuqin Zou
The electrochemical oxidation of 5-hydroxymethylfurfural (HMFOR) in alkaline electrolyte is a promising strategy for producing high-value chemicals from biomass derivatives. However, the disproportionation of aldehyde groups under strong alkaline conditions and the polymerization of HMF to form humic substances can impact the purity of 2,5-furandicarboxylic acid (FDCA) products. The use of neutral electrolytes offers an alternative environment for electrolysis, but the lack of OH − ions in the electrolyte often leads to low current density and low yields of FDCA. In this study, a sandwich-structured catalyst, consisting of Ru clusters confined between unilamellar MnO 2 nanosheets (S-Ru/MnO 2 ), was used in conjunction with an electrochemical pulse method to realize the electrochemical conversion of 5-hydroxymethylfurfural into FDCA in neutral electrolytes. Pulse electrolysis and the strong electron transfer between Ru clusters and MnO 2 nanosheets help maintain Ru in a low oxidation state, ensuring high activity. The increased *OH generation led to a groundbreaking current density of 47 mA/cm 2 at 1.55 V vs. reversible hydrogen electrode (RHE) and an outstanding yield rate of 98.7 % for FDCA in a neutral electrolyte. This work provides a strategy that combines electrocatalyst design with an electrolysis technique to achieve remarkable performance in neutral HMFOR.
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Nature Communications
·
2024
·Vol. 15
·期 1
·1-13
·
IF 14.7
Jia Hongnan,Yao Na,Jin Yiming,Wu Liqing,Zhu Juan,Luo Wei
Suppressing the kinetically favorable lattice oxygen oxidation mechanism pathway and triggering the adsorbate evolution mechanism pathway at the expense of activity are the state-of-the-art strategies for Ru-based electrocatalysts toward acidic water oxidation. Herein, atomically dispersed Ru species are anchored into an acidic stable vinyl-linked 2D covalent organic framework with unique crossed π-conjugation, termed as COF-205-Ru. The crossed π-conjugated structure of COF-205-Ru not only suppresses the dissolution of Ru through strong Ru-N motifs, but also reduces the oxidation state of Ru by multiple π-conjugations, thereby activating the oxygen coordinated to Ru and stabilizing the oxygen vacancies during oxygen evolution process. Experimental results including X-ray absorption spectroscopy, in situ Raman spectroscopy, in situ powder X-ray diffraction patterns, and theoretical calculations unveil the activated oxygen with elevated energy level of O 2 p band, decreased oxygen vacancy formation energy, promoted electrochemical stability, and significantly reduced energy barrier of potential determining step for acidic water oxidation. Consequently, the obtained COF-205-Ru displays a high mass activity with 2659.3 A g −1 , which is 32-fold higher than the commercial RuO 2 , and retains long-term durability of over 280 h. This work provides a strategy to simultaneously promote the stability and activity of Ru-based catalysts for acidic water oxidation.
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Science China-Chemistry
·
2025
·
IF 9.7
Qiu Zhuo,Dai Yiqi,Zhang Runzhi,Xiao Xin,Tong Yuqiao,Yao Lihua,Yan Dongpeng
Cost-effective metal-based electrocatalysts are desirable for industrial water and seawater electrolysis, triggering the hydrogen evolution reaction (HER) with high efficiency. Here, we report the loading of ultralow-content Ru-Os dual-atom onto NiCoP nanoneedles significantly enhancing HER in seawater splitting. The localization of 0.16% Ru and 0.58% Os atoms within NiCoP induces changes in the electronic structure and coordination environment of the Ni active sites. This catalyst achieves low overpotentials (29 and 303 mV in alkaline solution, 68 and 331 mV in alkaline seawater) at 10 and 800 mA/cm 2 , respectively, demonstrating remarkable stability by maintaining performance at 500 mA/cm 2 for 24 h in alkaline and simulated seawater. Experimental and theoretical studies indicate that ultralow content Ru and Os dual atoms are immobilized on the surface of NiCoP/NF through Ru-P and Os-P bonds, leading to electron transfer and changes in the coordination environment. These results enhance the activity of Ni active sits on support, demonstrating superior HER performance in alkaline solution and seawater. Ultralow content Ru and Os dual atoms in NiCoP@Ru-Os/NF play a crucial role in reducing the Gibbs free energy of hydrogen adsorption and lowering the d -band position of the catalyst, thereby accelerating the HER kinetic.
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ACS Sustainable Chemistry & Engineering
·
2025
·
IF 7.3
Shenghan Gao,Yuting Luo,Bo Li,Wen Cai,Huai Liu,Rui Zhang,Wenlong Jia,Lincai Peng
Modulating the electronic environment of single-atom metal catalysts is a promising yet challenging strategy to optimize their catalytic performance. Herein, electron-rich Ru single atoms were successfully confined within a CoOx matrix (Ru0.6CoOx) through a simple manual grinding-reduction strategy. The resulting Ru0.6CoOx catalyst demonstrated exceptional catalytic activity for the hydrogenolysis of 5-hydroxymethylfurfural (HMF) to 2,5-dimethylfuran (DMF), affording a nearly quantitative DMF yield with an impressive DMF productivity of 210.2 molDMF·mol–1Ru·h–1 at 160 °C. This productivity outperforms most of the noble metal-based catalysts for DMF production. Notably, Ru0.6CoOx also enabled the efficient conversion of HMF to DMF at a low reaction temperature of 120 °C or using a concentrated HMF solution (up to 20 wt %). Experimental studies combined with density functional theory calculations (DFT) revealed that the electronic interaction between the Ru species and CoOx generates electron-rich Ru single atoms, which serve as active sites to boost the H2 activation. Furthermore, the introduction of single Ru atoms was shown to increase the acidity of Ru0.6CoOx, thereby facilitating the cleavage of the C–OH bond during HMF hydrogenolysis. The boosted H2 activation ability and improved acidity of Ru0.6CoOx contribute significantly to its outstanding catalytic performance. This work provides valuable insights into the preparation of electron-rich single-atom metal catalysts for the catalytic hydrodeoxygenation of biomass-derived chemicals.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2025
·
IF 8.3
Jingwen Ma,Ruiting Wang,Tianai Zhang,Ying Tian,Jinhao Liu,Junbin Li
Urea-assisted hydrogen production is an emerging hydrogen production technology that offers a new approach to the efficient and clean production of hydrogen energy. The low energy consumption urea oxidation reaction replaces the high energy consumption oxygen evolution reaction (OER), significantly reducing the energy consumption of hydrogen production and achieving the resource utilization of pollutants in wastewater (including urea). It is expected to become an important pathway for green hydrogen production with both economic and environmental benefits. The novel composite catalyst Ru/NiMoOx@NC, prepared by supporting ruthenium on a nitrogen-doped carbon-coated nickel-molybdenum oxide support, exhibits highly efficient bifunctional catalytic activity, enabling it to efficiently catalyze the hydrogen evolution reaction (HER) and promote the urea oxidation reaction (UOR). Specifically, the introduction of trace ruthenium synergizes with the nickel-molybdenum bimetallic oxide to accelerate H 2 generation. The nitrogen-doped carbon substrate enhances the catalyst's electrical conductivity. Additionally, the incorporation of Mo reduces CO poisoning of Ni active sites during the UOR, further to enhance the catalyst's stability. By varying the loading of Ru, materials with optimal and superior properties are obtained. The Ru/NiMoO x @NC catalysts demonstrate excellent UOR (1.37 V vs. RHE@25 mA cm −2 ; 1.39 V vs. RHE@100 mA cm −2 ) and HER (−98 mV@25 mA cm −2 ) performance under alkaline conditions. The current density of the Ru/NiMoOx@NC electrode remains almost unchanged after cyclic voltammetry (CV) tests and chronoamperometric durability tests, exhibiting excellent catalytic stability. In this system, Ru/NiMoOx@NC serves as both the anode and cathode of the urea-assisted hydrogen production battery, which only requires a voltage of 1.56 V to achieve an output current density of 50 mA cm −2 and demonstrates excellent overall water electrolysis stability. This work provides new insights for the design of bifunctional catalysts for urea-assisted hydrogen production.
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CHEMICAL ENGINEERING SCIENCE
·
2025
·
IF 4.3
Fengjuan Liu,Yan Zhang,Tingting Wang,Peng Jiang,Bei Liu,Yunxia Wen,Ning Qu,Jie Kong,Zhenchen Tang,Feng Zeng,Han Lin,Xiaohua Lu,Tuo Ji,Jiahua Zhu
The strong N N bond, notoriously difficult to dissociate, has long posed a significant challenge to ammonia synthesis under mild conditions, typically requiring high temperatures and pressures. Here, Ru-supported Sr-based perovskite/CNT core/shell composites were developed as microwave-responsive catalysts for ammonia synthesis. Leveraging their exceptional microwave responsiveness, Ru/SrCeO 3 /CNT achieved an NH 3 production rate of 1.04 mmol·(g·h) −1 at 300 °C and 0.1 MPa, with no deactivation observed after 72 h. The energy consumption reached 0.10 MJ·(mol·g) −1 at 30 W much lower than the recent research on microwave ammonia synthesis. The core/shell architecture facilitated in-situ heat generation from the CNT core, enhancing interfacial reactions on Ru nanoparticles. Furthermore, XPS and H 2 -TPR analyses revealed that oxygen vacancies and strong interfacial interactions in the SrCeO 3 support boosted the electron-donating capacity of Ru active sites, promoting N N bond cleavage. This work offers a scalable, energy-efficient strategy for sustainable ammonia production.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Zeyi Guan,Liuyan Zhang,Yiqi Xie,Danting Wu,Binkai Yuan,Lichan Wu,Gengzhe Shen,Guibin Tan,Fujian Guo
Alkaline water electrolysis is recognized as an environmentally sustainable approach for generating high-energy-density clean hydrogen. However, its efficiency remains largely limited by the sluggish kinetics water dissociation in the hydrogen evolution reaction (HER), the challenge of activating water molecules, and the excessive consumption of OH − and high adsorption energy barriers of oxygenated intermediates during the oxygen evolution reaction (OER). In this work, A nanoneedle-structured Ru-NiCo₂O₄-Se electrocatalyst was developed, demonstrating excellent bifunctional electrocatalytic performance for both HER and OER. Through a combination of experimental characterizations and theoretical simulations, it had been revealed that the sharp-tip nanoneedle morphology generates intense local electric fields. These fields facilitate the enrichment of K + ions at the cathode, optimized the interfacial water structure, and substantially lower the energy barrier required for water dissociation. At the anode, the tip effect facilitated OH − accumulation, enhanced reactant mass transport, and accelerated OER kinetics. Moreover, metal–support interactions (MSI) between Ru nanoclusters and the support effectively modulate the adsorption behavior of H* and oxygenated intermediates, further boosting catalytic performance. The catalyst achieves overpotentials as low as −48 mV for HER and + 231 mV for OER at a current density of 10 mA·cm −2 , and delivers a high overall water splitting current of 100 mA·cm −2 at a cell voltage of only 1.7 V, along with remarkable long-term durability over hundreds of hours. This study presents an innovative strategy based on interfacial microenvironment engineering and electronic structure modulation, paving a fresh pathway for the development of cost-effective, high-performance, and long-lasting bifunctional electrocatalysts tailored for clean energy conversion.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2025
·
IF 8.5
Jiaoyang Wang,Qingtao Zeng,Kaile Cao,Yanshuai Cui,Haiyan Xiao,Longgang Wang
Organophosphorus pesticides (OPs) pose a significant threat to food safety due to their high toxicity and tendency to bioaccumulate. Conventional detection methods are constrained by reliance on specialized equipment and complex procedures, hindering rapid, on-site screening. In this study, a green synthesis approach was employed using hawthorn polysaccharide (HP) as a natural stabilizer to fabricate bimetallic Pd@Ru nanozymes (HP-Pd m Ru n NPs). The synergistic effect between palladium and ruthenium markedly enhanced the nanozymes' peroxidase-like catalytic activity and stability. Their catalytic behavior followed typical Michaelis–Menten kinetics, exhibiting a strong affinity for the substrate 3,3′,5,5′-tetramethylbenzidine (TMB). A colorimetric biosensor based on HP-Pd 10 Ru 20 NPs enabled rapid and sensitive detection of glyphosate, with a detection limit as low as 0.179 ng/mL and a linear range of 0.0002–200 μg/mL. The biosensor demonstrated excellent selectivity and recovery, offering promising potential for bioanalytical applications and contributing to the development of environmentally friendly, cost-effective technologies for detecting OPs residues.
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Energy & Environmental Materials
·
2025
·
IF 14.1
Jia Wang,De Wang,Zhenyu He,Mengyu Yan,Yinyu Xiang,Huipeng Li,Lina Xu,Junsheng Li
Ruthenium-based catalysts are promising alternatives to platinum for the hydrogen evolution reaction (HER) due to their comparable activity and lower cost. However, their widespread application in alkaline water electrolysis is limited by insufficient stability and excessive hydrogen binding. Herein, the Ru@Co 3 O 4 nanosheets (Ru@Co 3 O 4 NSs) featuring dominant exposure of the Co 3 O 4 (111) facets and precise anchoring of Ru nanoclusters onto these planes were constructed. The interaction between Ru nanoclusters and the Co 3 O 4 (111) facets induces a downshift of the Ru d -band center, optimizes the interfacial water network, and simultaneously prevents the leaching of Ru species. Ru@Co 3 O 4 NSs deliver exceptional alkaline HER performance, with an overpotential of 9.8 mV at 10 mA cm −2 and robust durability over 1000 h at 1 A cm −2 . The catalyst also achieves a price-normalized activity of 145.9 A $ −1 , nearly nine times that of commercial Pt/C. When applied in an anion exchange membrane water electrolyzer (AEMWE), Ru@Co 3 O 4 NSs reveal a low cell voltage of 1.93 V at 1 A cm −2 and operate stably for 60 h with a minimal degradation rate of 0.67 mV h −1 . This work provides a promising approach for designing low-cost, high-performance Ru-based catalysts for sustainable hydrogen production.
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