ACS Catalysis
·
2026
·
IF 13.6
Feiyang Zhang,Jun Li,Xin Cui,Kaixuan Wang,Zhuoming Wei,Weili Shi,Yu Guo,Yuxiang Song,Yonglong Li,Huatian Xiong,Shaoqi Zhan,Licheng Sun,Biaobiao Zhang
Abstract We report a porphyrin-bridged Ru(bda) coordination polymer integrated with carbon nanotubes, constructed from the well-defined homogeneous water oxidation catalyst in acid. The porphyrin linker simultaneously provides redox activity and proton-buffering functionality, enabling acidic water oxidation at an ultralow Ru loading (0.021 mgRu·cm–2). The resulting composite reaches current densities up to 200 mA·cm–2 in acid, exceeding previously reported molecular water oxidation catalyst-based anodes by one to two orders of magnitude. At identical metal loadings, it also outperforms both RuO2 and IrO2 benchmarks in both activity and stability. Electrochemical, spectroscopic, and theoretical results support porphyrin protonation and reversible oxidation, suggesting that ligand redox activity, together with proton management, contributes to the enhanced catalytic performance. These findings underscore the transformative potential of ligand engineering in molecular integration strategies for advancing artificial photosynthetic energy conversion systems.
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Analytical Methods
·
2025
·Vol. 17
·期 25
·5298-5307
·
IF 2.6
Yang Cao,Chun Huang,Kui Li,Xi Zhang,Mengfei Tong,Jiale Tu,Kun Yang,Shuai Yuan,Hong Zhang
To sensitively detect ochratoxin A (OTA), a CRISPR/Cas12a-assisted electrochemiluminescence (ECL) aptasensor based on COF@Ru coupled with a DNA tetrahedral scaffold (DTS) was successfully fabricated. The covalent organic framework (COF) acted as a confined micro-reactor for the tris(2,2′-bipyridyl)ruthenium(II)/tri-n-propylamine (Ru(bpy)32+/TPrA) system and hence, evidently enhanced ECL signals. Au nanoparticles (AuNPs) coupled with DTS caused more ferrocene (Fc)-modified quenching DNA probe molecules to be attached to the surface of the sensing electrode, which could reduce the detection background. Activated CRISPR/Cas12a could effectively amplify the ECL signal since it could cut off a considerable amount of quenching DNA probe molecules and make them move away from the electrode. Owing to these strategies, the fabricated ECL aptasensor could detect OTA as low as 3.5 fg mL−1 in a linear detection range of 10−5–100 ng mL−1. Furthermore, the CRISPR/Cas12a and COF@Ru coupled with DTS-based ECL biosensor possessed high stability and specificity. More importantly, the ECL biosensor could effectively detect OTA in food samples, indicating that it can play a role in monitoring OTA levels in the field of food safety.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Daniel Kobina Sam,Zhen Tang,Yan Cao
Noble-metal-based electrocatalysts have long been the top choice for hydrogen evolution reaction (HER) electrocatalysts, offering low overpotentials and Tafel slopes. Nonetheless, their use in alkaline media has been limited due to the sluggish kinetics of the Volmer process. Herein, we develop a unique biomass-derived heteroatom-doped porous carbon material via self-templating to anchor ruthenium‑molybdenum carbide (Ru-Mo 2 C) nanoclusters. The synthesized Ru-Mo 2 C-supported heteroatom-doped porous carbon (RuMo-NPCSPC) shows exceptional electrocatalytic ability for alkaline HER, achieving low overpotentials of 49, 85, and 92 mV to realize 10 mA cm −2 in 1 M KOH, alkaline seawater, and simulated alkaline seawater, respectively. The RuMo-NPCSPC also boasts low Tafel slopes and ultrahigh Faradaic Efficiencies (98–100 %) in alkaline media, outperforming most noble metal-based catalysts and mercantile Pt/C. Most importantly, the catalyst demonstrates outstanding stability, signifying its potential for industrial hydrogen production. This work delivers profound perspectives into synthesizing advanced nanostructured porous carbon materials using abundant biomass resources for alkaline HER.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Huiying Liao,Huihui Zhang,Xinjia Wei,Xiuge Zhao,Ji Ding,Ning An,Pengfei An,Sheng Dai,Zhenshan Hou
Converting carbon dioxide into high-value chemicals through catalytic means is one of the most promising approaches for CO 2 utilization. In this work, the ionic porous polymer-supported Ru single-atom catalysts were constructed for CO 2 hydrogenation reactions. It is noteworthy that the anions of the polymers exerted a significant influence on porosity and CO 2 adsorption capacity, which are crucial for achieving efficient CO 2 hydrogenation under mild conditions. Especially, the products of CO 2 hydrogenation on the polymer catalyst can be switched by tuning the type of amines, i.e. , with the assistance of tertiary amine, CO 2 /H 2 and methanol can produce methyl formate efficiently. However, CO 2 /H 2 , the primary and secondary amines switched to afford the corresponding formamides by N-formylation reaction with the identical catalyst. The detailed characterization demonstrates that Ru is only partially coordinated with phosphine ligand tethered in the polymer framework, while the remaining uncoordinated free phosphine bearing lone-pair electrons can activate CO 2 through a synergistic interaction with the moiety of ionic liquids, thereby enhancing the catalytic activity. The catalytic system exhibits high efficiency, stability and ease of recyclability, allowing for reuse up to ten times.
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Advanced Sustainable Systems
·
2020
·Vol. 4
·期 10
·1900136
·
IF 4.869
Xing Zhang,Hui Yan,Lingjun Zhu,Tian Li,Shurong Wang
The monomers and dimers produced via lignin depolymerization are a promising alternative to transportation fuels after hydrodeoxygenation (HDO). However, these compounds contain numerous oxygen-containing functional groups that are strongly bonded to aromatic rings. Therefore, the conventional HDO of lignin-derived compounds faces serious problems of catalyst deactivation due to coke deposition and low hydrocarbon yields. A metal–solid super acid catalyst, i.e., Ru(SO 4 2− )/ZrO 2 –CeO 2 , is synthesized, characterized, and evaluated for the HDO of various lignin-derived monomers and dimers in a biphasic n -dodecane/H 2 O system. A high cyclohexane yield of 98.5% is obtained by the HDO of phenol performed at 200 °C and 5 MPa. The “hydrated” configuration can be formed between the hydrogenation intermediates and H 2 O on the Ru sites. In addition, the anionic vacancies of ZrO 2 –CeO 2 can be occupied by H − derived from the heterolytic cleavage of H 2 , leading to the formation of metal hydrides. The strong acidity of SO 4 2− /ZrO 2 –CeO 2 is beneficial for the subsequent deoxygenation of the hydrotreated products. In addition, the biphasic system can minimize the side reactions induced by the strong acidity of the catalyst. The catalytic system also exhibits a good catalytic performance for the HDO of other lignin-derived monomers and dimers to produce cycloalkanes.
研究领域:
化学工程
·
催化科学
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2026
·
IF 9.6
Lixin Su,Shengnan Zhou,Di Liu,Shaokun Zhang,Songtao Zhang,Wenting Li,Mohsen Shakouri,Huan Pang
The kinetics of hydrogen oxidation reaction (HOR) in alkaline media is sluggish, exhibiting a decline by several orders of magnitude in comparison to that in acidic media. While Ru presents a cost-effective alternative to benchmark Pt with comparable hydrogen binding energy and enhanced oxophilicity, its performance is limited by excessive hydroxyl (OH*) adsorption under alkaline conditions. Generally, the metal-organic framework (MOF)-derived catalytic structure facilitates high dispersion of active sites, enabling effective interfacial synergy. Herein, MOF-derived Ru-based catalysts were constructed by dispersing Ru sites onto transition metal oxide/carbon supports (Ru-MO x /C, M = V, Mn, Fe, Co). Among them, the constructed Ru-VO x /C achieves superior HOR performance under both acidic and alkaline conditions, and possesses the minimal acid-base kinetic gap. Experimental and theoretical analyses reveal that the prominent performance originates from interfacial charge redistribution and microenvironment modulation, induced by d-d orbital coupling and built-in electric field at the Ru-VO x interface, which synergistically optimizes and balances the key intermediate (H ⁎ , OH*, and H 2 O) behaviors. Remarkably, the oxophilic VO x species could create a local OH − -enriched microenvironment that mitigates excessive OH* adsorption on Ru sites while ensuring efficient supply of reactive species, thereby synergistically modulating the diverse intermediate behaviors and enhancing HOR performance.
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FUEL
·
2020
·
IF 5.578
Jing-Pei Cao,Tao Xie,Xiao-Yan Zhao,Chen Zhu,Wei Jiang,Ming Zhao,Yun-Peng Zhao,Xian-Yong Wei
Selective hydrogenolysis, the aromatic ether C-O bonds under mild conditions, is crucial for the valorization of lignin. In this context, the effects of H 2 and solvent on the hydrogenolysis of lignin model compounds over Ru catalysts were explored. With H 2 as hydrogen donor, the Ru/AC exhibited the highest activity for converting lignin model compounds into monomeric compounds, whereas H 2 led to low selectivity of aromatics. However, isopropanol was the good H-donor solvent, which could provide a large amount of active hydrogen to promote the cleavage of C-O bonds. Additionally, the yield of aromatics in isopropanol was higher than that under H 2 atmosphere. It could be ascribed to the fact that isopropanol is the protic solvent which displays Lewis basicity, and is a good H-bond donor and a good H-bond acceptor. The higher electron-releasing inductive effect of isopropanol made it easier to provide active hydrogen. Based on the experiments, the mechanism of benzyl phenyl ether hydrogenolysis in H 2 and isopropanol system was presented.
研究领域:
化学工程
·
催化科学
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Huiqun Cao,Bin Liang,Shenghua Ye,Ziqiong Zhuang,Lirong Zheng,Wenda Chen,Weibin Chen,Jie Zhang,Qinghao Zhang,Jianhong Liu,Xueqing Yan,Qianling Zhang
Conversion of NO 3 − -to-NH 3 via the electrocatalytic nitrate reduction reaction (NO 3 - RR) is an emerging strategy for ammonia production and storage of “green hydrogen”, but is limited by the dissatisfactory activity and selectivity. In this study, we discovered that cobalt carbonate hydroxide (Co 2 (OH) 2 CO 3 ) underwent a potential-induced self-reconstruction to cobalt hydroxide (Co(OH) 2 ) during NO 3 - RR. The incorporation of Ru into Co 2 (OH) 2 CO 3 expedited the aforementioned self-reconstruction process and resulted in the formation of Ru single-atomic sites (Ru SASs) anchored on Co(OH) 2 nanosheets. This structure is reported as a highly efficient electrocatalyst for NO 3 − -to-NH 3 conversion and exhibits exceptional electrochemical performance in zinc-NO 3 − batteries. Theoretical analysis revealed that the conversion of NO 3 − -to-NH 3 occurred on Ru SASs through an N-end pathway with *NO as a characteristic intermediate. Furthermore, Ru SASs facilitated the thermodynamic-determining step of *NH 2 -to-*NH 3 , thus promoting the overall NO 3 − -to-NH 3 conversion process.
研究领域:
材料科学
·
电化学
·
催化化学
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Reaction Chemistry & Engineering
·
2026
·
IF 2.9
Wenjing Guo,Qing Zhao,Yadong Bi,Kailin Wang,Mengming Wang,Baozhen Wu,Xinli Tong
A series of metal oxide promoters were incorporated into the Ru/C catalyst by the impregnation method. Notably, the addition of ZnO demonstrated a pronounced promoting effect on the hydrogen-transfer reductive catalytic fractionation (RCF) of poplar wood. The 1 wt% Ru/ZnO/C catalyst achieved a total phenolic monomer yield of 34.2 %, even surpassing the commercial 5 wt% Ru/C catalyst despite its lower Ru loading. This enhancement stems from the synergistic interaction between ZnO-derived Lewis acid sites and Ru metal nanoparticles. Furthermore, the influences of key parameters such as reaction temperature, catalyst dosage, molar ratio of ZnO to Ru and solvent on the RCF activity were systematically investigated. During recycling process, the Ru/ZnO/C catalyst exhibited gradual deactivation, accompanied by an increased proportion of unsaturated phenolic monomers in the product distribution, indicating a decline in hydrogenation capacity. The deactivation behavior of the Ru/ZnO/C catalyst was characterized using BET, XPS, TEM, and ICP techniques, and tentative regeneration attempts were employed on the spent catalyst.
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FUEL
·
2026
·
IF 7.8
Miao Ma,Min Yang,Cai-Yue Zhang,Hai-Yi Sun,Rong-Jing Su,Xiao-Rui Yue,Chen-Xi Li,Yong-Ming Chai,Bin Dong
Developing low-cost, high-performance Ru-based hydrogen evolution reaction (HER) catalysts is crucial for advancing anion exchange membrane water electrolysis (AEMWE) technology. In this study, based on the Sabatier principle, a Ru/CoMoO 4 heterojunction catalyst with a ternary “nanorod-macroparticle-microparticle” structure is designed. Benefiting from the strong electronic interactions, a lower d-band center of Ru/CoMoO 4 is observed, resulting in optimal adsorption between Ru species and the key H* intermediates to greatly enhance the hydrogen desorption kinetics. Importantly, this interface engineering effect prevents the Volmer-Tafel step from becoming rate-limiting step, thereby promoting electron and mass transport. As a consequence, Ru/CoMoO 4 outperforms most of the reported HER catalysts at an ultra-low Ru loading of only 0.2 wt%. In alkaline media, it only requires an overpotential of 55 mV to achieve 100 mA cm −2 , with a low Tafel slope of 16 mV dec -1 , and operates stably for over 230 h at an industrial-grade current density of 1000 mA cm -2 . The AEMWE electrolyzer based on the Ru/CoMoO 4 catalyst achieves efficient and stable hydrogen production at 1000 mA cm⁻ 2 @ 1.93 V. This work not only provides a high-performance catalyst, but also elucidates a strategy for precisely controlling d-band center through heterojunction interface engineering to optimize reaction [email protected]
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JOURNAL OF HAZARDOUS MATERIALS
·
2018
·
IF 6.434
Xiaolong Liu,Li Chen,Tingyu Zhu,Ruliang Ning
Catalytic oxidation of chlorobenzene over noble metal catalysts Pd/TiO 2 , Pt/TiO 2 , Ru/TiO 2 , and Rh/TiO 2 was evaluated, and Ru/TiO 2 contributed the highest catalytic activity and CO 2 selectivity. During the oxidation, polychlorinated benzenes PhCl x (x ≥ 2) were observed, and Ru/TiO 2 showed apparently lower PhCl x concentrations than other three samples. With the improvement of temperature, the maximum concentration appeared in the sequence of dichlorobenzene (PhCl 2 ), trichlorobenzene (PhCl 3 ), tetrachlorobenzene (PhCl 4 ), and pentchlorobenzene (PhCl 5 ), whereas the concentration of hexachlorobenzene (PhCl 6 ) was always low and showed no apparent regularity. Besides, the dioxin-like PCBs (dl-PCBs) were collected and analyzed for Pd/TiO 2 and Ru/TiO 2 . The ∑dl-PCBs produced by Pd/TiO 2 (0.0055 ng WHO-TEQ/Nm 3 ) was about 1.5 times that of Ru/TiO 2 (0.0027 ng WHO-TEQ/Nm 3 ). XPS analyses revealed that Ru/TiO 2 -used and Rh/TiO 2 -used gave the lowest and the highest Cl content of 0.61% and 1.87%. Ru/TiO 2 -used afforded the lowest (Cl ad +Cl or )/Cl value (22.1%) and the highest Cl br /Cl value (77.9%), which might be an important reason for its strongest chlorine removal ability and the lowest yields of polychlorinated by-products, whereas other three catalysts showed similarity in the Cl distributions. Additionally, systematic in-situ FTIR studies were conducted, and a reaction mechanism for the catalytic oxidation of chlorobenzene was proposed.
研究领域:
环境化学
·
催化
·
污染控制
·
材料科学
·
化学工程
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CHINESE JOURNAL OF CATALYSIS
·
2026
·
IF 17.2
Xu Yu,Han Tian,Ziyi Yu,Fantao Kong,Min Wang,Ruxiang Shen,Xiangzhi Cui,Jianlin Shi
A dual-site synergistic catalytic mechanism is proposed to optimize the OHad binding energy (OHBE) by constructing ultrafine Ru nanoclusters modified with highly oxygenophilic WO 2.72 clusters in nitrogen-doped carbon carriers, which can optimize the adsorptions of OH ad and active hydrogen species, respectively, resulting in a marked increase in hydrogen oxidation reaction (HOR) activity. The constructed Ru-WO 2.72 -NC shows a HOR mass activity about 8 times that of Pt-C, and the corresponding alkaline exchange membrane fuel cells demonstrate rather higher peak power densities than Ru-NC with 1.193 W cm –2 and more than 1 W cm –2 in H₂ fuel and CO/H 2 mixtures, respectively. The excellent alkaline HOR performance of Ru-WO 2.72 -NC is attributed to the adsorption of OH ad species by WO 2.72 clusters, which synergizes with the adsorption and dissociation of hydrogen on Ru to facilitate the Volmer step. The success in constructing dual-site synergistic catalysis of Ru-WO 2.72 -NC anode provides valuable insight and new guidelines for designing and studying high-activity alkaline HOR catalysts.
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