ACS Sustainable Chemistry & Engineering
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2026
·
IF 7.3
Shiyu Huang,Yinze Yang,Yan Du,Pengxiao Wei,Yafei Zhao,Huishan Shang,Dan Wang,Dongyang Li,Bing Zhang
A bifunctional Cu/CeO2/halloysite catalyst was rationally constructed via strong electrostatic adsorption to enable switchable conversion of furfural into either furfuryl alcohol or isopropyl furfuryl ether. Highly dispersed Cu nanoparticles are anchored on CeO2 nanoislands supported by acid-etched halloysite nanotubes, creating a unique “support–adjuvant–active site” synergy. This architecture facilitates H2 activation and tandem hydrogenation–etherification, allowing precise temperature-controlled pathway selection. Under mild conditions, furfural hydrogenation to furfuryl alcohol proceeds via a low-energy barrier (0.9 eV) with a stable intermediate, whereas etherification requires overcoming a significant barrier (1.6 eV), becoming favorable only at elevated temperatures. In situ FTIR, kinetic studies, and DFT calculations reveal the mechanistic origin of this selectivity. The catalyst displays high activity, tunable selectivity, and robust recyclability, providing a versatile strategy for controlling reaction pathways in the valorization of biomass-derived platform molecules.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2023
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IF 4.2
Shan Zhang,Binbo Jiang,Mingliang Tong,Yao Yang,Zuwei Liao,Zhengliang Huang,Jingyuan Sun,Jingdai Wang,Yongrong Yang
Cost-effective heterogeneous catalysts are critical to the ketonization of carboxylic acids for producing biofuels and platform chemicals. Herein, nanocrystalline Cu-loaded CeO2 with 1.0–9.0 wt % Cu loadings was synthesized by the precipitation-impregnation method, in which 3.0 wt % Cu/CeO2 exhibits the best performance of 72% acetone yield at 330 °C, 97% 3-pentanone yield at 360 °C, and 86% 4-heptanone yield at 400 °C, with good durability up to 10 h on stream. Detailed analyses reveal that 3.0 wt % Cu/CeO2 has the highest percentage of O-vacancy sites, more moderate acid–base sites, and better capacity to adsorb and activate carboxylic acids. In situ DRIFT spectra indicate that monodentate, bridging bidentate, and chelating bidentate modes coexist when carboxylic acid is dissociatively adsorbed on 3.0 wt % Cu/CeO2. Based on the above investigations, we propose a mechanism over 3.0 wt % Cu/CeO2 through the β-ketoacid intermediate route, which gives more details to help future research into the design and development of catalysts for ketonization.
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Science Advances
·
2026
·Vol. 12
·期 13
·
IF 13.9
Yu Zhang,Ningqiang Zhang,Yiwei Liu,Haofan Lei,Tao Zhou,Wenlong Wu,Wei-Wei Wang,Han Yan,Chao Ma,Ken-ichi Shimizu,Chun-Jiang Jia,Jie Zeng
For oxide-supported metal catalysts, metal-support interaction (MSI) facilitates metal dispersion at the expense of the metallic character, resulting in a trade-off between active site utilization and intrinsic activity. Here, we used a thermal aging strategy to modulate the MSI in Cu/CeO 2 catalysts, facilitating the formation of metallic Cu sites upon H 2 reduction while maintaining metal dispersion. Systematic experiments confirmed that thermal aging at 800°C lowered the reduction temperature and increased the reduction degree of Cu sites. Microscopy evidenced few-atom-layered Cu nanoclusters before and after H 2 reduction, whereas in situ spectroscopy revealed metallic Cu nanoparticles under H 2 atmosphere. This discrepancy indicated a reversible structural evolution from aggregation to redispersion in thermally aged Cu/CeO 2 . The catalytic activity for acetylene semihydrogenation was unlocked on metallic Cu sites, compared to nearly inactive Cu sites in conventional Cu/CeO 2 counterparts. Our work developed an effective strategy for rational modulation of MSI, offering the feasibility to tailor-make active sites for specific reactions.
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ADVANCED FUNCTIONAL MATERIALS
·
2025
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IF 19
Lei Xiong,Xianbiao Fu,Jun Zhang,Shuang Liu,Shanshan Li,Shaojie Lu,Dong Wang,Qin Yue
Cu shows unique characteristics for electrochemical CO 2 reduction reaction (CO 2 RR) to hydrocarbons and oxygenates due to the moderate adsorption energy of the key intermediate *CO. However, it remains a challenge to selectively control CO 2 RR towards C 1 (e.g., CH 4 ) or C 2+ (e.g., C 2 H 4 and C 2 H 5 OH) through simple interface engineering. Herein, a series of inverse catalysts, composed of CeO 2 nanoparticles over Cu substrate (Cu-CeO 2 -x), are subtly designed to tackle the issues. It is verified CeO 2 decoration induces highly active Cu/CeO 2 interfacial sites that enhance the adsorption and conversion of CO 2 and *CO intermediates into C 2+ or CH 4 , while the Cu sites are conducive to *CO generation. With the increase of CeO 2 deposition, the C 2+ and CH 4 selectivity present a volcano-type and increasing tendency with maximum faradic efficiency of 62.6% and 51.3%, respectively. In-situ infrared spectroscopy and theoretical calculations reveal that moderate CeO 2 loading allows the Cu/CeO 2 interfacial sites to cooperate efficiently with the Cu sites to promote the coupling of *CO/*CHO intermediates, thus enhancing the C 2+ selectivity. In contrast, excessive CeO 2 loading suppresses the C─C coupling but boosts unilaterally the hydrogenation, thus promoting the CH 4 production. This work provides effective strategies to regulate the CO 2 RR selectivity by modulating metal/oxide interfaces.
研究领域:
材料科学
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电化学
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催化科学
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Chemical Science
·
2019
·Vol. 10
·期 12
·3556-3566
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IF 9.556
Yanan Liu,Alan J. McCue,Pengfei Yang,Yufei He,Lirong Zheng,Xingzhong Cao,Yi Man,Junting Feng,James A. Anderson,Dianqing Li
The impregnation method is commonly employed to prepare supported multi-metallic catalysts but it is often difficult to achieve homogeneous and stable alloy structures. In this work, we revealed the dependence of alloying behavior on the support morphology by fabricating Ni–Cu over different shaped CeO2. Specifically, nanocube ceria favoured the formation of monometallic Cu and Ni-rich phases whereas polycrystalline and nanorod ceria induced the formation of a mixture of Cu-rich alloys with monometallic Ni. Surprisingly, nanopolyhedron (NP) ceria led to the generation of homogeneous Ni–Cu nanoalloys owing to the equivalent interactions of Ni and Cu species with CeO2 (111) facets which exposed relatively few coordinative unsaturated sites. More importantly, a strong interfacial effect was observed for Ni–Cu/CeO2-NP due to the presence of CeOx adjacent to metal sites at the interface, resulting in excellent stability of the alloy structure. With the aid of CeOx, NiCu nanoalloys showed outstanding catalytic behaviour in acetylene and hexyne hydrogenation reactions. This study provides valuable insights into how fully alloyed and stable catalysts may be prepared by tailoring the support morphology while still employing a universal impregnation method.
研究领域:
催化化学
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材料科学
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PubMed
高影响因子
MICROCHEMICAL JOURNAL
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2025
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IF 5.1
Lulu Cui,Weijie Shi,Houshen Li,Xiuxian Zhao,Shiyun Ai,Xiangju Meng,Shuhong Sun,Zeyi Guo
For bimetallic nanozymes, the closeness between the two elements is closely related to their properties, but achieving tight contact between the two components still faces challenges. Herein, copper was introduced by the coordination effect between the organic ligand in Ce-MOF and Cu 2+ , then a series of Cu-CeO 2 nanozymes were obtained by thermal treatment. The content of copper can be easily controlled and the spindle-shaped structure assembled by multilayer flakes can be obtained. The total antioxidant capacity (TAC) detection program based on the excellent peroxidase (POD)-like activity of the as-prepared Cu-CeO 2 nanozyme showed a wide linear detection range and ideal detection limits for ascorbic acid (AA), glutathione (GSH), Trolox and cysteine (Cys). More importantly, this method can be applied in TAC detection of commercial samples. This work provided a method for the design of high performance bimetallic nanozymes and developed a sensor that can be applied to detect TAC in vitamin C tablets and beverages.
研究领域:
材料科学
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生物医学工程
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分析化学
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Science Bulletin
·
2025
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IF 21.1
Qingyu Wang,Yangyang Wan,Qichen Liu,Yida Zhang,Zhentao Ma,Zirui Xu,Pengting Sun,Gongming Wang,Hai-Long Jiang,Wenping Sun,Xusheng Zheng
Photocatalytic urea production from nitrogen (N 2 ) and carbon dioxide (CO 2 ) is a sustainable and eco-friendly alternative to the Bosch-Meiser route. However, it remains a significant challenge in developing highly efficient photocatalysts for enhancing C-N coupling to high-yield urea synthesis. Herein, we propose a multi-site photocatalyst concept to address the concern of low yield by simultaneously improving photogenerated carrier separation and reactant activation. As a proof of concept, a well-defined multi-site photocatalyst, Ru nanoparticles and Cu single atoms decorated CeO 2 nanorods (Ru-Cu/CeO 2 ), is developed for efficient urea production. The incorporation of Ru and Cu sites is crucial not only to generate high-density photogenerated electrons, but also to facilitate N 2 and CO 2 adsorption and conversion. The in situ formed local nitrogen-rich area at Ru sites increases the encounter possibility with the carbon-containing species generated from Cu sites, substantially promoting C-N coupling. The Ru-Cu/CeO 2 photocatalyst exhibits an impressive urea yield rate of 16.7 μmol g −1 h −1 , which ranks among the best performance reported to date. This work emphasizes the importance of multi-site catalyst design concept in guaranteeing rapid C-N coupling in photocatalytic urea synthesis and beyond.
研究领域:
化学工程
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材料科学
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环境科学
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PubMed
高影响因子
Journal of Materials Research and Technology-JMR&T
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2022
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IF 6.267
Lihua Li,Shuang Liu,Meng Zhou,Yi Zhang,Shengli Liang,Jinliang Huang,Baohong Tian,Yongfeng Geng,Yijie Ban,Yong Liu,Yanlin Jia,Xu Li,Alex A. Volinsky
The effect of graphene on the thermal deformation of Cu/CeO 2 /Cr and GO-Cu/CeO 2 /Cr composites was studied. The isothermal compression test was carried out with Gleeble-1500D thermomechanical simulation device in the range of 600–900 °C and strain rate of 0.001–1 s −1 . The microstructure after deformation was characterized and analyzed by optical microscope, scanning electron microscope (SEM), transmission electron microscope (TEM) and electron backscatter diffraction (EBSD). The interaction of work hardening, dynamic recovery and dynamic recrystallization was described. The constitutive equation was successfully established. The results show that Cr particles are extruded into strips, and nano CeO 2 particles nail dislocations, which inhibit dynamic recovery and dynamic recrystallization. Dispersion strengthening, twin strengthening and grain refinement strengthening occur the thermal deformation of GO-Cu/CeO 2 /Cr composites, increase the flow stress and activation energy of the composites, and inhibit the dynamic recrystallization of the composites. When the hot deformation temperature increases, the texture orientation is strengthened. GO-Cu/CeO 2 /Cr composites have typical dynamic recovery characteristics and high temperature properties.
研究领域:
材料科学
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纳米技术
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高影响因子
Carbon Capture Science & Technology
·
2023
·
IF 0
Bowen Lu,Fan Wu,Xiaoshan Li,Cong Luo,Liqi Zhang
The interfacial structure of metal and oxide support plays a pivotal role in reverse water gas shift (RWGS). However, rare work investigated the factor of the metal-oxide interface during RWGS reaction. In this work, the interface of Cu/CeO 2 catalysts was designed through the thermal treatment of copper nitrate salt on CeO 2 with an H 2 atmosphere under different temperatures, and CO 2 hydrogenation performance was studied at 400 °C to investigate the effect of interfacial structure on RWGS reaction. Among these prepared catalysts, Cu/CeO 2 -400 catalysts achieved the best CO 2 conversion activity (CO production rate 1.23 mol/g cat . h). Cu interacted with CeO 2 to form Cu-O-Ce interface and induced more oxygen vacancy formation. The oxygen vacancy around the Cu-CeO 2 interface enhanced CO 2 adsorption and promoted CO 2 conversion. CO 2 reacted with active hydrogen to COOH, then COOH species dissociated into CO and OH adsorbed on the surface of Cu-CeO 2 . These results gave insights into the design of a highly effective catalyst for CO 2 hydrogenation.
研究领域:
催化化学
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材料科学
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能源化学
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APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Jingjing Tan,Jing He,Kuan Gao,Shanhui Zhu,Jinglei Cui,Long Huang,Yulei Zhu,Yongxiang Zhao
The hydrogenation of furfural to furfuryl alcohol in liquid was performed over Cu/CeO 2 catalyst with different morphology that was nanorod (CeO 2 -R), nanocube (CeO 2 -C) and nanopolyhedron (CeO 2 -P), respectively. It was observed that the Cu/CeO 2 -R catalyst exposed (1 1 0) crystal plane owns more oxygen vacancies and metal sites of Cu 0 in comparison with the catalyst of Cu/CeO 2 -P and Cu/CeO 2 -C. Meanwhile, it exhibited superior catalytic performance for furfural hydrogenation to furfuryl alcohol with a high yield of 98 % at 100 °C, 2 MPa H 2 within 4 h. The structure–activity relationship demonstrated that the catalyst intrinsic activity (TOF) is positively related to the concentration of oxygen vacancies and the metal sites of Cu 0 on its surface. DFT calculations and in-situ FTIR confirmed that Cu/CeO 2 -R (1 1 0) catalyst with more oxygen vacancy is in favor of the adsorption and activation of furfural (C O) on the catalyst surface compared with Cu/CeO 2 -P (1 1 1) and Cu/CeO 2 -C (1 0 0). Accordingly, the remarkable efficiency of Cu/CeO 2 -R catalyst can be assigned to the synergistic catalysis between the surface Cu 0 and the oxygen vacancies. Cu 0 was used to adsorb and activate H 2 , whereas the oxygen vacancies facilitate the adsorption of C O by O on the surface of the catalyst.
研究领域:
催化化学
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材料科学
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2026
·
IF 9.1
Haihuan Sun,Xiaoyan He,Zongcheng Yang,Xiaoqing Dou,Wenhan Fan,Chengqing Yuan,Xiuqin Bai
Biofilm formation on material surfaces is a persistent challenge in aquatic environments, creating an urgent need for sustainable catalytic antimicrobial strategies. Although ceria nanozymes with haloperoxidase (HPO)-like activity have attracted increasing attention, their practical application is limited by the low density of surface Ce 3+ sites and oxygen vacancies. Herein, defect-engineered Cu-doped CeO 2 nanozymes were developed to enhance HPO-like catalytic activity and antibacterial performance. Cu incorporation regulated the Ce 4+ /Ce 3+ redox equilibrium and promoted oxygen-vacancy formation, resulting in enhanced catalytic activity, while controlled Cu 2+ release contributed to synergistic antibacterial effects. As a result, the optimized Cu-CeO 2 nanozymes achieved approximately 99% bacterial inactivation against E. coli and 97% inhibition against Bacillus sp. at a low nanoparticle concentration of 10 mg/L, demonstrating broad antibacterial activity against representative Gram-negative and Gram-positive bacteria. Combined experimental characterization and density functional theory calculations revealed the defect-mediated mechanism underlying the enhanced catalytic performance. This work provides a defect-engineering strategy for developing ceria-based nanozymes with enhanced catalytic antibacterial performance for potential catalytic antifouling applications.
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Catalysts
·
2026
·Vol. 16
·期 7
·628
·
IF 4.5
Shiqi Ma,Haoyang Li,Yuchen Huang,Kai Sun,Yuejia Huang,Yarong Fang,Yan Du
Selective catalytic oxidation of ammonia (NH3-SCO) is a promising technology for ammonia abatement. Cu/CeO2catalysts have attracted extensive attention because of their strong metal–support interaction and favorable redox properties. However, their practical application is still limited by insufficient low-temperature catalytic activity and unsatisfactory control of by-product formation. Herein, phosphate-functionalized Cu/CeO2catalysts were fabricated to regulate surface acidity and oxygen species behavior, thereby promoting low-temperature NH3-SCO activity. The optimal Acid-Cu/CeO2catalyst achieved 90% NH3conversion at 260 °C, corresponding to a 192 °C decrease in T90compared with pristine Cu/CeO2(452 °C). Kinetic analysis showed that the apparent activation energy decreased from 125.78 to 84.70 kJ mol−1after phosphoric acid modification. In addition, Acid-Cu/CeO2maintained relatively high N2selectivity and lower NOxselectivity over the tested temperature range, indicating that phosphate modification suppresses the deep oxidation of NH3to NOxby-products. Structural and surface characterization results demonstrated that Cu species remained highly dispersed on CeO2after modification, while surface phosphate species modified the local electronic environment and redistributed oxygen species. O 1s XPS and O2-TPD results revealed that phosphate modification decreased the static surface adsorbed/defect-related oxygen fraction but improved the accessibility and mobility of labile surface/subsurface or weakly bound lattice oxygen species. Py-IR and DRIFTS results further showed that phosphate modification increased Brønsted/Lewis acidity, enhanced NH3adsorption and N-H activation, and facilitated the formation and subsequent consumption of NHx/-NHO-related intermediates under reaction conditions. This work provides insights into phosphate-mediated regulation of surface acidity and oxygen mobility and offers a strategy for designing efficient low-temperature Cu/CeO2-based NH3-SCO catalysts.
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