JOURNAL OF MATERIALS SCIENCE
·
2024
·Vol. 59
·期 45
·21027-21039
·
IF 3.5
Zhang Peng,Guo Mengya,Wang Fujiang,Tang Qiong,Ge Hui,Guo Shuke,Zhou Ligong,Li Xuekuan,Dong Jinxiang,Tang Mingxing,Liu Lei
Selective hydrogenation is an effective approach to utilize coal tar and slurry oil to produce high value-added fine chemicals. However, how to efficiently improve the selectivity of the target product and the stability of the catalyst is difficult. Herein, the PdZn alloy catalyst was synthesized by the assistance of strong interaction between active metal (Pd) and support (ZnO) for hydrogenation of anthracene to symmetrical octahydro anthracene (sym-OHA). The PdZn alloy catalyst reduced at 400 °C was found to exhibit a 100% conversion of the anthracen with 84.77% selectivity to sym-OHA under the optimized conditions (200 °C, 1 MPa). The characterization analysis indicated that the PdZn alloy with electron-rich Pd active sites is more efficient in the selective hydrogenation than the pure Pd metal. The study of the deep hydrogenation of sym-OHA (Hydrogenation of sym-OHA to perhydroanhtracene) showed that PdZn alloy catalysts were inactive to further hydrogenation of sym-OHA. Additionally, due to the strong interaction between Pd and ZnO, the Pd/ZnO(400) catalyst shows high stability for five cycles. These findings are of practical significance for the selective hydrogenation of polycyclic aromatic hydrocarbons (PAHs) to produce high value-added products.
研究领域:
催化化学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
Nature Communications
·
2024
·Vol. 15
·期 1
·1-11
·
IF 14.7
Wang Pu,Zhang Xingyu,Shi Run,Zhao Jiaqi,Waterhouse Geoffrey I. N.,Tang Junwang,Zhang Tierui
The selective oxidative dehydrogenation of ethane (ODHE) is attracting increasing attention as a method for ethylene production. Typically, thermocatalysts operating at high temperatures are needed for C–H activation in ethane. In this study, we describe a low temperature ( < 140 °C) photocatalytic route for ODHE, using O 2 as the oxidant. A photocatalyst containing PdZn intermetallic nanoparticles supported on ZnO is prepared, affording an ethylene production rate of 46.4 mmol g –1 h –1 with 92.6% ethylene selectivity under 365 nm irradiation. When we employ a simulated shale gas feed, the photocatalytic ODHE system achieves nearly 20% ethane conversion while maintaining an ethylene selectivity of about 87%. The robust interface between the PdZn intermetallic nanoparticles and ZnO support plays a crucial role in ethane activation through a photo-assisted Mars-van Krevelen mechanism, followed by a rapid lattice oxygen replenishment to complete the reaction cycle. Our findings demonstrate that photocatalytic ODHE is a promising method for alkane-to-alkene conversions under mild conditions.
研究领域:
化学工程
·
材料科学
·
能源科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF CATALYSIS
·
2020
·
IF 7.888
Hongyu Yang,Kai Wang,Zhenghua Tang,Zhen Liu,Shaowei Chen
Despite the recent advances in preparing high-efficiency and durable electrocatalysts for oxygen reduction reaction (ORR) toward fuel cell applications , there is still lacking of the understanding regarding the relationship between the electrocatalytic performance and the surface structure of the catalyst at atomic level. Herein, three PdZn bimetallic composites named as PdZn_Disordered, PdZn_Ordered and Pd@Zn_Core-shell (Pd: Zn = 1: 1) were prepared for ORR in alkaline medium to examine the surface structure effects. Multiple characterization means revealed that PdZn_Disordered and PdZn_Ordered had amorphous PdZn and ordered PdZn alloyed structure, respectively, while Pd@Zn_Core-shell held a Pd-core-ordered and Zn-shell-disordered architecture. In the electrochemical ORR tests, Pd@Zn_Core-shell exhibited the superior activity and stability in the series, outperforming the Pd/C and Pt/C catalysts. The electrocatalytic performance followed the order of Pd@Zn_Core-shell > PdZn_Ordered » PdZn_Disordered, which can be attributed to the effects of different surface structures of the catalysts.
研究领域:
材料科学
·
电化学
·
能源科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF CATALYSIS
·
2017
·
IF 6.844
Lingfeng Shen,Shanjun Mao,Jianqing Li,Mingming Li,Ping Chen,Haoran Li,Zhirong Chen,Yong Wang
This work highlights a novel hybrid catalyst, intermetallic PdZn on CN@ZnO (PdZn/CN@ZnO), which serves as a highly efficient heterogeneous catalyst for semihydrogenation of 2-methyl-3-butyn-2-ol utilizing water as the solvent. Compared with intermetallic PdZn on ZnO (PdZn/ZnO), PdZn/CN@ZnO displays almost sixfold higher TOF while retaining high selectivity. It is assumed that the introduction of biomass-derived hydrophilic nitrogen-doped carbon into the ZnO helped to promote catalyst dispersion in aqueous media, ensuring better mass transfer. Further experiments and theoretical calculations showed that from Pd particles to intermetallic PdZn, the decrease of corner and edge Pd atoms might be a factor leading to the improvement of selectivity. Recycling experiments demonstrated that the PdZn/CN@ZnO catalyst could be reused at least eight times without significant decrease in activity or selectivity. Furthermore, when applied to industrially relevant alkenols that are building molecules for the production of vitamin E, the present catalyst still offered excellent performance. It is expected that the present catalytic system will demonstrate its high potential for practical production of vitamin E.
研究领域:
催化化学
·
材料科学
·
有机合成
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2019
·
IF 4.084
Zilong Zeng,Guoliang Liu,Jiafeng Geng,Dengwei Jing,Xinlin Hong,Liejin Guo
Methanol steam reforming (MSR) is deemed to be an effective way for hydrogen production and Pd/ZnO catalyst were found to exhibit high activity in this reaction. However, their activities are strongly related to the preparations methods. In most cases, these catalysts are synthesized by impregnation or co-precipitation methods, aiming to change the dispersion and stability of Pd nanoparticle to get better performance. Here we report an efficient Pd/ZnO catalyst that was synthesized with zeolitic imidazolate framework-8 (ZIF-8) as the precursor, on which Pd ions was supported after NaHB 4 reduction. Typically, when the catalyst reduced at 300 °C for 2 h, the methanol conversion could reach 97–98% and the CO 2 selectivity is around 86.3% under the reaction condition of 0.1 MPa, water/CH 3 OH = 1.2:1 (mol ratio), WHSV methanol = 43152ml/g cat *h, catalyst = 0.1 g, our catalyst was found to show much better performance than other Pd@ZnO catalysts prepared by other methods, especially in terms of selectivity which is particularly important for hydrogen fuel cell application considering that Pt electrode could be poisoned by even trace amount of CO. It turned out that the large surface area , enough holes, evenly distributed PdZn alloy activity sites and abundant oxygen vacancies lead to the overall excellent performance of our catalyst.
研究领域:
催化化学
·
材料科学
·
能源化学
✓ 已验证
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2018
·
IF 11.698
Yazhi Yin,Bing Hu,Xinliang Li,Xiaohai Zhou,Xinlin Hong,Guoliang Liu
Direct CO 2 hydrogenation to methanol provides a means of CO 2 fixation and a way of hydrogen storage in a more energy-dense and transportable form. Pd-ZnO catalysts can be active for this reaction, but their activities are strongly associated with the preparation methods which influence the dispersion and stability of Pd nanoparticle. Here we report a novel fabrication of highly effective PdZn alloy catalysts derived from Pd@zeolitic imidazolate framework (ZIF-8) for the hydrogenation of CO 2 . The confinement of subnanometric Pd particles in the pore framework of ZIF-8 facilitates the formation of Pd-ZnO interfaces with strong-metal-support-interaction (SMSI) after a simple pyrolysis under air condition. The porous texture and high surface area of ZnO ensures a high dispersion of Pd nanoparticles. Different pyrolysis temperatures were studied in catalysis and the highest methanol yield reached 0.65 g g cat −1 h −1 at 270 °C, 4.5 MPa, with a TOF of 972 h −1 , over a PdZn catalyst prepared at 400 °C. Such excellent activity has ranked the top reported values over advanced Pd-based catalysts under comparable conditions. The crucial factors for such high methanol yield are the formation of small-sized PdZn alloy particles after H 2 reduction and abundant surface oxygen defects on ZnO. The SMSI between PdZn and ZnO also ensures a long term stability of our PdZn catalysts. At last, we propose the active site that was strongly associated with methanol formation is a PdZn alloy rather than metallic Pd.
研究领域:
催化化学
·
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2023
·
IF 6.2
Mingzhi Chen,Sifan Zhang,Chenyu Zhu,Huan Zhang,Lihua Zhu,Yingliang Feng,Jiexiang Wang,Qian Yang,Bingqian Liu,Wentao Xu
MOFs (metal-organic frameworks) materials have been widely applied in sensing and catalysis, with the advantages of large surface area, numerous active sites, controllable size and morphology. Herein, we report the preparation of the caged PdZn/NC catalysts with the PdZn alloy nanoparticles on carbon doping with nitrogen owing high electrocatalytic performance by using a hydrothermal synthesis and pyrolysis strategy. The caged structure and PdZn alloy are demonstrated by a series of advanced characterization techniques. The material combines the advantages of bimetallic alloy and MOFs cage structure to realize highly efficient electrocatalytic oxidation of ethanol oxidation reactions (EOR) and methanol oxidation reactions (MOR) simultaneously. Electrochemical test results show that PdZn/NC-2 has a mass activity of 2.41 A mg −1 pd and 2.64 A mg −1 pd for methanol and ethanol oxidation, respectively, which is 12.68 times (MOR) and 14.67 times (EOR) higher than that of commercial Pd/C. This is probably attributed to the cage-like structure of PdZn/NC separating the Pd nanoclusters , resulting in high Pd dispersion. Simultaneously, the electronic property of Pd is adjusted after the formation of the complete PdZn alloy, improving the desorption of the carbon-based intermediates from the Pd active sites. This increases the CO poisoning resistance, resulting in good alcohol electrocatalytic oxidation activity and stability.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Xueying Wang,Wendong Wang,Jingru Li,Yegang Xia,Jinxin He,Dongren Cai,Juanjuan Bian,Guowu Zhan
Developing efficient PdZn/ZnO catalysts for the thermal hydrogenation of CO 2 to methanol remains challenging. In this study, the supported PdZn/ZnO catalysts were fabricated by depositing Pd metalloporphyrin ( viz. , TCPP(Pd)) precursor on Zn-Al layered double hydroxides (ZA-LDH) or the derived Zn-Al layered double oxides (ZA-LDO), whereby the effects of the preparation method, Pd loading amounts, and reduction temperatures on the nanostructure and catalytic performance of PdZn/ZnO catalysts were thoroughly examined. The optimized catalyst, 3.28 %Pd@ZA-LDO-R400, with PdZn particle size of 20 nm exhibited superior CO 2 conversion of 8.1 %, methanol space–time yield (STY MeOH-Pd ) of 15 g MeOH g Pd − 1 h −1 , and good stability during 100 h on stream at 300 °C and 3 MPa. Notably, the crystal structures of the PdZn alloy, specifically the PdZn α and PdZn β , were significantly influenced by the reduction temperature. As the reduction temperature increased, the PdZn α phase transformed into the PdZn β phase. Density functional theory (DFT) calculations confirmed that PdZn β has a lower energy barrier for H 2 dissociation compared to PdZn α , thereby enhancing catalytic activity. Furthermore, in-situ DRIFTS characterization revealed that CO 2 hydrogenation to methanol over the PdZn/ZnO catalyst predominantly follows the formate pathway, with key species including HCOO* and CH 3 O*. The hydrogenation of HCOOH* to CHO* was identified as the rate-limiting step in this reaction. Accordingly, this study offers an effective method for fabricating intermetallic PdZn β catalysts with improved performance in CO 2 hydrogenation.
研究领域:
催化化学
·
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Yang Sun,Fan Yang,Siyuan Sun,Hongchen Liu,Yankun Sun,Na Ta,Yongfeng Li
The anodic precious metal catalyst of direct methanol fuel cell (DMFC) is poisoned due to CO adsorption, which makes the methanol oxidation reaction (MOR) kinetics tardily. In this study, a series of hierarchical core–shell structure catalysts PdZn/ZDC@SiO 2 were synthesized by loading PdZn nanoparticles (NPs) on ZIF-8 derived porous carbon (ZDC) and protecting by the mesoporous silica (SiO 2 ) are reported. A hierarchical core–shell structure informed in PdZn/ZDC@SiO 2(20) caused by mesoporous silica shell leads to well-dispersed and uniform of PdZn NPs (10 nm). Compared with commercial palladium carbon (Pd/C), the optimized catalyst PdZn/ZDC@SiO 2(20) has higher current density (765.2 mA/mg) and stronger CO toxicity tolerance (I f /I b = 3.30). And the onset potential and the peak potential of PdZn/ZDC@SiO 2(20) (−0.294 V, −0.203 V) are more negative in CO stripping experiment. Silica is an inorganic oxide that can provide oxygen-containing species to the adjoining precious metal sites and promote CO oxidation. In addition, PdZn NPs can accelerated electron transport and then improve methanol oxidation performance due to the changing electronic structure of Pd and the modifying the surface adsorption of the catalyst. PdZn/ZDC@SiO 2(20) is a potential substitute material for noble metal catalyst that can be used for direct methanol fuel cells.
研究领域:
材料科学
·
电化学
·
能源催化
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Hugang Zhang,Xinmiao Li,Yile Wang,Kai Deng,Hongjie Yu,You Xu,Hongjing Wang,Ziqiang Wang,Liang Wang
Two-dimensional (2D) Pd-based materials have been extensively researched as a cathode for oxygen reduction reaction (ORR) due to its distinctive physicochemical characteristics. In this paper, we report the controllable construction of porous wrinkled PdZn bimetallene (PdZn BMene) with the lattice distortions and grain boundaries via a one-step hydrothermal approach. Benefiting from the curved 2D metallene morphology, more sufficient and exposed active sites, and synergistic effect of alloy components, the resultant PdZn BMene exhibits outstanding ORR performance in 0.1 M KOH electrolyte, with the mass activity of 1.11 mA μg Pd −1 , which is 1.6, 6.4, and 21.6 times higher than those of Pd metallene (0.43 mA μg Pd −1 ), commercial Pt/C (0.15 mA μg Pd −1 ), and Pd/C (0.049 mA μg Pd −1 ), respectively. Moreover, PdZn BMene also possesses commendable durability, with only 7.2% activity loss after 30,000 potential cycles and a 5.3% attenuation of current density after 10-h durability test. Meanwhile, the assembled zinc-air battery with PdZn BMene as cathode catalyst possess an open-circuit voltage of 1.5 V and a maximum power density of 108.7 mW cm −2 along with benign durability. The present study highlights the advances of 2D Pd-based alloy bimetallene for realizing high-performance against the ORR application.
研究领域:
材料科学
·
电化学
·
催化科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Ziyi Li,Xiaolong Zhu,Jiamu Xiao,Wei Lu,Donglin Gan,Jian Shen,Xuefeng Jiang,Mingqian Wang
The misuse of antibiotics exacerbates the problems of bacterial resistance, rendering antibiotic treatment ineffective and, in severe cases, posing life-threatening risks. Therefore, the development of novel antimicrobial materials and their clinical applications have garnered significant attention from healthcare professionals. Bimetallic nanozymes hold significant potential for treating clinical bacterial infections, owing to their superior antimicrobial activity and excellent biocompatibility. In this study, PdZn and PdCu bimetallic nanozymes with folded structures were synthesized using a one-step hydrothermal method. Their photothermal and peroxidase-like catalytic activities were compared, and the underlying causes of the variations in their catalytic performance were analyzed through computational studies. Additionally, the antimicrobial efficacy and wound-healing potential of these two nanozymes were evaluated. Experimental results demonstrated that PdCu exhibited superior catalytic performance compared to PdZn, which aligned with density functional theory calculations confirming its enhanced catalytic ability. In vitro antimicrobial experiments have successfully demonstrated that PdZn and PdCu can effectively inhibit the survival of Escherichia coli and Staphylococcus aureus down to less than 2 % by utilising the synergistic effect of photo-thermal catalysis at 980 nm near-infrared laser. Antibacterial experiments in vivo demonstrated that PdZn and PdCu nanozymes could promote wound healing and slow down the inflammatory response. PdCu exhibited a superior ability to promote wound healing compared with PdZn. PdCu + H 2 O 2 + NIR and PdZn + H 2 O 2 + NIR decreased the trauma area to 9.37 % and 6.04 % respectively, whereas the control group decreased it to only 41.21 %. Overall, this study further explores the potential of Pd-based nanozymes for biological applications and provides guidance for the synthesis of highly efficient Pd-based 2D nanobiomaterials.
研究领域:
生物医学
·
材料科学
·
纳米医学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2025
·
IF 6.3
Wenjun Kang,Jiabao Chen,Yuanjie Zhang,Yajie Guo,Fanpeng Meng,Konggang Qu,Rui Li,Lei Wang,Zongge Li,Haibo Li
The fabrication of ordered noble metal alloys on carbon supports can effectively alter the electronic structure of the catalyst interface and the valence states of the elements, presenting a viable alternative to platinum (Pt) for the electrocatalysis of the oxygen reduction reaction (ORR) in metal–air battery cathodes. Herein, we developed a straightforward in situ reduction synthesis method that facilitates the formation of ordered PdZn alloy catalysts on hollow carbon under specific conditions, optimizing ORR efficiency. In an oxygen-saturated 0.1 M KOH solution, the ORR performance of the synthesized Pd 0.02 Zn-NC-900 catalyst exhibits an initial potential of ∼0.996 V and a half-wave potential of ∼0.887 V at 1600 rpm. When integrated into a zinc–air battery, it achieves a remarkable specific power of 213.7 mW cm −2 and a specific capacity of 813.8 mAh g Zn − 1 , outperforming commercial Pt/C. Our research focuses on the efficient synthesis of carbon-supported ordered PdZn alloys to address the needs of electrochemical energy conversion applications.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）