CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Shimin Chen,Junnan Han,Zhihuan Li,Zijie Lin,Min Wang,Hucheng Song,Xiaodong Pi,Dongke Li,Linwei Yu,Jun Xu,Kunji Chen
Lithium-carbon dioxide (Li-CO 2 ) batteries using high ion-conductive inorganic molten salt electrolytes, as a kind of promising carbon–neutral technology, have attracted much attention due to the high safety and high energy density. However, sluggish CO 2 reduction reaction (CO 2 RR) and evolution reaction (CO 2 ER) kinetics at cathodes make these batteries losing most of their capacity and power. Here, by engineering the carbon-free three-dimensional (3D) Cr-N-Ru catalysts on silicon nanopillars (Si NP) cathodes, we report a reversible solar photothermal (SPT) molten salt Li-CO 2 battery where solar energy can be efficiently harvested (over 90 % absorption rate from 300 nm to 2500 nm), concentrated and converted to heat. Theoretical simulations support that the 3D Cr-N-Ru catalysts exhibit lower energy barrier and more effectively catalyze the CO 2 RR and CO 2 ER process compared to individual Ru or CrN catalyst. The SPT Li-CO 2 battery shows a reversible cycle lifespan of 83 cycles with lower charge potential (3.2 V) and higher energy efficiency of 72 %, corresponding to ∼ 0.9 V potential gap, than the one using conventional Ru catalysts assembled on Si NP cathode. This battery technology paves the way for developing the next-generation safe and high-energy–density energy storage batteries with carbon–neutral effect.
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ANALYST
·
2014
·Vol. 139
·期 18
·4613-4619
·
IF 3.906
Dan Zhang,Ai Gao,Yang Xu,Xue-Bo Yin,Xi-Wen He,Yu-Kui Zhang
Mesoporous silica nanoparticles (MSNs) were co-doped with Gd3+ and Al3+ and then loaded with Ru(bpy)32+ by ion-exchange to prepare Ru/Gd–Al@MSNs. The as-prepared Ru/Gd–Al@MSNs were applied as contrast agents for in vivo fluorescence and magnetic resonance (MR) dual-modality imaging with a mouse as a model. The effects of Al3+ and MSNs on longitudinal relaxivity (r1) and fluorescence were investigated using a series of Gd-containing silica nanoparticles, including Gd@MSNs, Gd–Al@MSNs, and Ru/Gd–Al@nonporous silica nanoparticles. Co-doping with Al3+ improved the loading of Gd3+; the mesoporous structure improved the water exchange rate. The improvement enhanced the MR imaging efficiency of the Ru/Gd–Al@MSN probe. A higher relaxivity (19.2 mM−1 s−1) was observed compared to that from a commercial contrast agent, Gd-diethylene triamine pentaacetic acid (Gd-DTPA). Importantly, the mesoporous structure provided a large specific surface area for the loading of Ru(bpy)32+ by a simple ion-exchange procedure. Intense red fluorescence was observed from Ru/Gd–Al@MSN probes. The versatility of Ru/Gd–Al@MSNs for dual-modality imaging was demonstrated using in vivo fluorescence imaging and T1-weighted MR imaging with a mouse model. The nanoparticles are biocompatible and may be attractive for clinical applications.
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Russian Journal of Physical Chemistry A
·
2022
·Vol. 96
·期 9
·1944-1950
·
IF 0.791
Zhang Yuanyang,Bao Kun,Wang Xuchao,Wang Linqi
Abstract A series of Ru and Ru–Pd supported samples on deep desulfurization, especially thiophene-like compounds, were prepared by wet impregnation method. It indicated that the suitable Ru content on the support could be 1.5 wt % (Ru(1.5)/Al 2 O 3 ) under used experimental conditions. The effects of Pd on Ru(1.5)/Al 2 O 3 sample showed that the suitable content of Pd was probably 0.3 wt % (Ru(1.5)–Pd(0.3)/Al 2 O 3 ), and its breakthrough sulfur capacity could be reached to 1.244 g S /kg Cat . XPS and SEM characterization over fresh and used samples of Ru(1.5)–Pd(0.3)/Al 2 O 3 indicated that it had good stable structure. Furthermore, it indicated that the adsorption isotherm model of Freundlich equation was well fitted the experimental data ( R 2 = 0.989) and the parameters of Freundlich equation were obtained by linear regression.
研究领域:
催化化学
·
环境工程
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GREEN CHEMISTRY
·
2026
·
IF 10.6
Danni Liu,Kaige Zhang,Wenli Zhao,Xiaopo Niu,Xiangwen Zhang,Qingfa Wang
To address the challenges of complex separation and high energy consumption in producing high-density biofuels from biomass, developing high-efficiency bifunctional catalyst to integrate carbon-carbon coupling and hydrodeoxygenation processes is highly desired. Herein, a bifunctional catalyst with RuOx anchored on the edge of NbOPO4 nanosheets was successfully fabricated through an impregnation-calcination method, enabling one-pot solvent-free conversion of lignin-derived phenol and benzyl alcohol into polycycloalkane perhydrofluorene. The NbOPO4 nanosheet edges were enriched in oxygen vacancies and were prone to anchoring RuOx species preferentially. The optimized 3%RuOx/NbOPO4 exhibited abundant Ru-O-Nb interfacial species, which synergized with Brønsted acid sites (BASs) to enhance the alkylation performance. The in-situ generated Ru0 species from the Ru-O-Nb interfacial species exhibited superior hydrogen dissociation capability, then the synergistic interaction with BASs through hydrogen spillover significantly boosted the hydrodeoxygenation efficiency. 3%RuOx/NbOPO4 with more Ru-O-Nb interfacial species exhibited high conversion of benzyl alcohol (98%) and yield towards perhydrofluorene (72%) under mild conditions (160 °C, 3 h) with a low environmental E-factor (≤2.8). Mechanistic studies identified the cyclization hydrogenation of oxygenated intermediates as the rate-determining step, and the product dicyclohexylmethane was mainly formed from the selective ring opening of perhydrofluorene over the synergy metal-acid sites of 3%RuOx/NbOPO4. This study provides a deep insight into designing efficient bifunctional catalysts for sustainable aviation fuel production through process integration.
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ACS Catalysis
·
2026
·
IF 13.6
Xuan Zhao,Jinni Shen,Xiang Li,Rongqi Xu,Lei Bai,Li Zhu,Shuai Yang,Aiyang Wang,Shulin Wang,Man Xu,Xianliang Fu
Abstract Modulating cocatalyst loading and its concomitant structural evolution represents a key strategy for optimizing the photocatalytic hydrogen evolution reaction (HER). However, a quantitative investigation into the loading-dependent evolution of active sites, its kinetic impacts on the H2 evolution rate (rH2), and the inherent trade-off between atomic utilization and cocatalyst stability remains elusive. Herein, a library of over twenty Ru/CdS nanorod samples with gradient loadings (0.009–2.88%, wt %) was constructed via a one-pot solvothermal method. By introducing the relative enhancement coefficient (ke) and marginal promotion rate (ηm), the influence of Ru site evolution on HER performance was investigated from both macroscopic cumulative and microscopic instantaneous perspectives. A distinct three-stage nonlinear evolutionary profile was revealed for the HER with increasing Ru content. Specifically, according to the ηm results, at the initial low-loading stage (<0.03%), positive cooperativity occurs among neighboring Ru single atoms, resulting in a quadratic increase in HER activity. Despite maximizing Ru utilization, these single-atom sites undergo progressive structural reconstruction during continuous operation, leading to a decay in activity. As the loading amount enters the coalescence transition regime [0.03–0.20%], reduced Ru atom-utilization efficiency and the parasitic light-shielding effect drag ηm into a sharp exponential decay, thereby attenuating the acceleration of rH2. Further increasing the loading amount [0.25, 2.88%] drives Ru site transition to nanoparticles, and a saturation plateau is subsequently approached due to an accentuated light-blocking effect and the conversion of active sites into carrier recombination centers. Although nanoparticle sites compromise Ru atom efficiency, they deliver enhanced durability, revealing a trade-off between atomic efficiency and catalytic lifespan. These findings demonstrate that, rather than merely maximizing rH2 by tuning the cocatalyst amount, more effort should be devoted to enhancing the critical loading amount of neighboring robust single-atom Ru cocatalysts. Overall, this work develops an alternative paradigm for cocatalyst evaluation and underscores the urgent imperative to develop robust neighboring single-atom catalysts for highly efficient solar-to-hydrogen conversion.
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ChemCatChem
·
2026
·Vol. 18
·期 5
·e01665
·
IF 4.1
Weimi Ding,Guoshuai Fu,Ruiqi Xu,Yifan Li,Guowei Yang,Shuang Li,Pu Liu
Developing efficient and durable oxygen evolution reaction (OER) electrocatalysts is essential for scalable hydrogen production via water splitting. While NiFe-layered double hydroxides (LDHs) are promising low-cost catalysts, their catalytic performance and stability remain limited. In this study, we report a one-step laser ablation in liquid (LAL) strategy to synthesize low-loading Ru-doped NiFe-LDH nanosheets (NiFeRu/C-LDH) with precisely controlled electronic and structural properties. The laser-driven uniform incorporation of Ru 4 + into the NiFe-LDH lattice induces contraction and optimization of the local coordination environment. The resulting catalyst achieves low overpotentials of 236 and 299 mV at 10 and 100 mA cm − 2 , respectively, in 1 M KOH, outperforming commercial IrO 2 and undoped NiFe/C-LDH. It also demonstrates high durability with 95.3% activity retention after 200 h of continuous operation. Combined experimental and Density functional theory (DFT) calculations, the theoretical analyses reveal that strong Ru–O coordination and enhanced electronic interactions activate adjacent Fe sites, and establish a Fe–Ru dual active center configuration that facilitates OH − adsorption and lowers the energy barrier of the rate-determining O–O coupling step. This work offers a scalable laser-based synthesis route for high-performance electrocatalysts with tailored active sites.
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JOURNAL OF CATALYSIS
·
2025
·
IF 6.5
Zhen Zhang,Quanxiao Dong,Yingqi Cui,Dan Wu,Armin Rezayan,Tianliang Lu,Renfeng Nie,Xiaoqin Si,Jianshe Wang,Chunbao Xu,Yongsheng Zhang
Catalytic oxidative depolymerization of lignin is an important strategy for producing valuable oxygen-functionalized monoaromatic compounds. However, this process is less efficient over heterogeneous catalysts due to the slow rate-determining step of selective oxidation of secondary alcohol (C α -OH to C α =O) in β-O-4 lignin linkages. Herein, a facile and efficient Ru(OH) x /C catalyst was developed for the oxidative depolymerization of lignin model compounds and real lignin in aqueous phase using molecular oxygen as oxidant. Extensive characterizations revealed that molecular oxygen abstracts electrons from the conductive carbon matrix to generate superoxide radicals (•O 2 – ), which are subsequently converted to hydroperoxide radicals (HOO•) in the presence of water. The C α -OH in the β-O-4 linkages first reacts with Ru-OH to form a Ru-O-C(H)- metal alkoxide intermediate, which then undergoes β-H elimination with the help of HOO• to generate H 2 O 2 and surface Ru-O-C•- species. Hydrolysis of Ru-O-C•- leads to the generation of C α =O products and the regeneration of Ru-OH sites. Different from the traditional Ru(OH) x -catalyzed alcohol dehydration mechanism in which Ru abstracts β-H to form Ru-H, in this case, the β-H in the Ru-alkoxide intermediate is eliminated by the hydroperoxide radicals rather than Ru, avoiding the formation of inert Ru-H species, thereby accelerating the dehydrogenation of C α -OH to C α =O. Electrochemical measurements further confirmed the charge transfer from Ru(OH) x to carbon during alcohol oxidation, demonstrating that electron donation by alcohol occurs on Ru(OH) x , while electron abstraction by O 2 occurs on the carbon. The free-radical-involved β-H elimination reaction pathway endows Ru(OH) x /C with superior catalytic oxidation activity in the aqueous phase compared with traditional metal oxides supported Ru(OH) x (e.g. SiO 2 , Al 2 O 3 , TiO 2 ), and provides a fundamental basis for the rational design of aqueous phase oxidation catalysts.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2017
·Vol. 43
·期 3
·1355-1364
·
IF 3.582
Jin Yang,Zhenkai Cui,Jiantai Ma,Zhengping Dong
Cotton, which has abundant oxygen-containing hydrophilic groups , can adsorb a lot of water or other water soluble materials . In this paper, cotton was impregnated in CoCl 2 aqueous solution. Co 2+ can be uniformly adsorbed on cotton fibers . After been freeze-dried, the Co 2+ -adsorbed cotton was carbonized under an inert atmosphere and the Co nanoparticles (NPs) modified cotton derived carbon fibers (Co/CCF) were obtained. The Co/CCF was then dispersed in RuCl 3 aqueous solution, so that Ru 3+ can be reduced by metallic Co NPs through spontaneous replacement reaction and covered on Co NPs surface . Hence, the Ru@Co/CCF catalyst was prepared with low Ru loading in the view of Ru saving. In the catalytic hydrolysis of ammonia borane (NH 3 ·BH 3 , AB), the Ru@Co/CCF catalyst showed excellent catalytic activity as compared with Ru/CCF and many other noble metal based catalysts . The superior activity of the catalyst is mainly due to the highly dispersed Ru@Co NPs on the carbon fibers and the uniform covering of the metallic Ru on the surface of Co NPs. Moreover, owing to the magnetic core of the Ru@Co NPs, Ru@Co/CCF catalyst can be easily separated from the reaction system using an external magnetic field . Thus, this work provided a useful strategy for facile preparation of low precious metals loading catalysts using cheap and environmental starting material as catalyst support precursor material .
研究领域:
催化化学
·
氢能
·
纳米材料
·
可持续化学
·
材料科学
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2026
·
IF 3.9
Fang-Jing Liu,Meng-Jie Wang,Shan-Shan Gao,Lei Xia,Yao Lu,Mei Zhong,Xiao Zhou,Xian-Yong Wei,Yun-Peng Zhao
A promising strategy for lignin valorization is catalytic hydrogenolysis (CH) of C–O or C–C bridging bonds over supported metal catalysts to produce aromatics. Herein, a bimetallic RuNi/CeO2 catalyst was developed via impregnation and evaluated for CH of alkali lignin and its model compounds. Comprehensive catalyst characterizations confirmed the strong synergistic Ru–Ni nanoparticles, abundant oxygen vacancies (Ov), and moderate-to-strong acid sites on RuNi/CeO2. It achieved 100% conversion of benzyl phenyl ether (BPE) under mild conditions (100 °C and 1.5 MPa H2) with toluene and phenol as the main products, markedly outperforming monometallic counterparts. It also exhibited excellent performance for other α-O-4 and β-O-4 model compounds under moderate conditions of 180 °C and 0.5 MPa H2, affording aromatic monomers as the dominant products. Mechanistic studies indicated that RuNi/CeO2 cooperatively activates H2 and isopropanol to generate hydrogen radicals (H•) and protons (H+), facilitating selective cleavage of C–O bonds. Applied to alkali lignin, CH over the catalyst produced a 41.1 wt % lignin oil, with phenols constituting over 70% of the liquid products, underscoring its efficacy in real lignin conversion. This work provides an efficient and selective catalytic strategy for lignin valorization, contributing to the sustainable production of valuable aromatics in the biorefining industry.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Fuguang Liu,Zhonghan Feng,Xinyue Zhang,Liang Cui,Jingquan Liu
The creation of inexpensive, high-performance catalysts to reduce the overpotential of the oxygen evolution reaction (OER) process is critical for the electrolysis of water for hydrogen production. Therefore, we applied a one-step hydrothermal method using cation exchange reaction (CER) to prepare Fe-doped and interfacial Ru nanoclusters co-engineered Ni(OH) 2 nanosheets directly grafted on Ni foam (Ru@Fe-Ni(OH) 2 /NF) for OER process. Results of electrochemical tests reveal that Ru@Fe-Ni(OH) 2 /NF has excellent OER activity, and its overpotential (η) is only 266.4 mV when the current density is 50 mA cm −2 in 1 M KOH solution, even lower than that of commercial OER catalyst RuO 2 (355 mV). The Tafel slope also decreases from 133.8 mV dec −1 for pristine Ni(OH) 2 /NF material to 24.1 mV dec −1 for Ru@Fe-Ni(OH) 2 /NF, indicating the higher charge transfer rates and fastest kinetics for water oxidation. At an overpotential of 300 mV the optimal turnover frequency (TOF) of 0.062 s −1 for Ru@Fe-Ni(OH) 2 /NF is achieved compared to that of Ni(OH) 2 /NF (0.014 s −1 , NN), demonstrating the fast reaction kinetics of the as-prepared electrocatcalyst. After 24 h stability test, the catalytic activity of Ru@Fe-Ni(OH) 2 /NF was only attenuated by 2 %, showing excellent OER stability and durability. Our results show that we have successfully developed an efficient OER catalyst for green and efficient electrocatalytic hydrolysis to produce H 2 and O 2 , providing a promising method for clean H 2 production.
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CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Lifang An,Jie Fan,Buhuan Wang,Jingyi Yang,Guolian Wang,Meng Zhang,Zhongyi Liu
Ru/Fumed SiO 2 achieves 100% DMT conversion and 100% DMCD selectivity. • Macropores of Fumed SiO 2 lower diffusion barriers and enhance active site utilization. • Strong Ru-O-Si interaction promotes Ru dispersion and ensures 5-cycle reusability. • Low apparent activation energy enables high-efficiency aromatic ring hydrogenation. The growing accumulation of waste polyethylene terephthalate (PET) causes severe resource depletion and environmental pollution, making its high-value chemical recycling essential for sustainable development. PET methanolysis affords dimethyl terephthalate (DMT), and its selective hydrogenation to dimethyl 1,4-cyclohexanedicarboxylate (DMCD) connects waste PET valorization with high-performance polyester synthesis. Herein, a series of Ru-based catalysts supported on microporous-dominated S-1, ordered mesoporous MCM-41 and SBA-15, and Fumed SiO 2 with the open interparticle macro-mesoporous were prepared by the incipient wetness impregnation, and the role of support pore structure in DMT hydrogenation to DMCD was systematically examined. The results show that the open interparticle macro-mesoporous framework of Fumed SiO 2 alleviates diffusion constraints and improves the accessibility of Ru active sites. This structure enables uniform Ru dispersion, giving Ru/Fumed SiO 2 the smallest average Ru particle size (6.0 nm). Surface Si-OH groups anchor Ru species through Ru-O-Si interfacial structures, which strengthens metal-support interactions and promotes H 2 activation and active-site utilization. Under 180 °C, 3.0 MPa H 2 , and 3 h, Ru/Fumed SiO 2 delivers 100% DMT conversion and 100% DMCD selectivity. It also shows the lowest apparent activation energy (39.0 kJ·mol −1 ), stable performance over five cycles, and over 93% conversion and selectivity for representative substituted aromatic compounds. These findings demonstrate that an open interparticle macro-mesoporous framework could improve molecular accessibility, mitigate mass-transfer limitations, and enhance hydrogenation efficiency. Download: Download high-res image (185KB) Download: Download full-size image
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Materials Horizons
·
2023
·Vol. 10
·期 12
·5712-5719
·
IF 13.3
Mengmeng Wang,Yunmei Du,Shuangshuang Li,Xiaoli Sun,Bin Li,Yuanxiang Gu,Lei Wang
The N-doping strategy plays a vital role in optimizing electrocatalytic performance, but it often requires high-temperatures accompanied by the emission of irritating gases, which is contrary to the concept of energy saving and environmental protection. Based on this, this work innovatively uses the quenching of waste heat and the non-equilibrium state of materials to realize controllable N-doping. Notably, N dopants stimulate metal-like electroconductivity and accelerate the alkaline HER kinetics by optimizing the electronic structure of Ru2P. Surprisingly, the hydrophilic Ru core and the N-Ru2P shell with a low HER reaction energy barrier synergistically expedite hydrogen release. As anticipated, the current density of N-Ru2P@Ru (963 mA cm−2) is 2.6-fold that of Pt/C (359 mA cm−2) at 150 mV. Overall, the novel N-doping technology greatly simplifies material preparation procedures and reduces energy consumption. Moreover, this unique N-doping strategy provides a new idea for optimizing the catalyst structure and reaction kinetics.
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