Russian Journal of Physical Chemistry A
·
2024
·Vol. 98
·期 7
·1495-1504
·
IF 0.7
Siyong Zhao,Deng Jie,Li Zhangjie,Chen Yongdong
The three-way catalysts (TWC) are required to have high thermal stability and excellent catalytic activity. The MgAl 2 O 4 spinel is a thermal stable material, but its reactivity is unsatisfactory. In this work, CeO 2 was used as a promoter to modify MgAl 2 O 4 spinel, and the cerium modified MgAl 2 O 4 spinel (MAC) was applied as the carrier to construct PdCu/MAC catalyst. The catalytic activity evaluation showed that modifying MgAl 2 O 4 spinel with a handful of cerium (0.12 mol-Ce/mol-Mg) dramatically improved the three-way catalytic activity, especially for the elimination of NO x and C 3 H 8 . The XRD and XPS proved that these cerium cations incorporated into spinel lattices and occupied Al sites. For this reason, the cerium in PdCu/MAC-1 is mainly in +3 valence (Ce 3+ /Ce = 60.2%), which is accompanied by the formation of abundant oxygen vacancies (45.9%). These factors significantly promoted the dispersion of PdCu nanoparticles, and thus strengthened metal-support interaction, consequently the enhanced catalytic performance. However, adding excessive cerium (0.24 mol-Ce/mol-Mg) resulted in negative effect. This might be related to the appearance of isolated CeO 2 crystal originating from the separate nucleation of excessive cerium cations. This work provides some guidance for developing TWC with both high thermal stability and activity.
研究领域:
催化化学
·
材料科学
·
环境化学
✓ 已验证
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2019
·
IF 5.155
Xiaozhi Guo,Hongyuan Shang,Jun Guo,Hui Xu,Yukou Du
Constructing efficient catalysts for the electrooxidation of fuels is of vital importance for realizing the commercialization of fuel cells. Unfortunately, most of catalysts (e.g. Pt) suffer from limited activity and poor durability for the electrooxidation of liquid fuel . Also, the drawbacks of extremely high cost and nature scarcity have also severely hindered their large-scale applications. Here, we demonstrated the synthesis of a new class of well-defined and three-dimensional (3D) flower-like nanocatalysts which assembled by ultrafine two-dimensional (2D) alloyed PdCu nanosheets . Structurally, the as-obtained PdCu alloy nanoflowers (NFs) possessed high surface area with abundant surface active sites. Benefiting from the unique structural properties and the strong alloy effect, the as-obtained PdCu NFs can display greatly enhanced performances toward ethylene glycol oxidation reaction (EGOR) with the mass/specific activity of 4714.1 mA mg −1 /13.7 mA cm −2 , which are 4.4 and 6.85 times of Pd/C catalysts, respectively. Most strikingly, such 2D nanosheets-constructed 3D nanoflower-like structure also enables the PdCu catalysts with high long-term stability for EGOR. As a proof of concept, this work not only presents the rational design and construction of catalysts with well-defined structure for the fuel cells reactions but also provides a promising method to largely promote the electrochemical performances of catalysts.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2019
·
IF 6.361
Ping'er Yu,Hui Xu,Liujun Jin,Chunyan Chen,Hongyuan Shang,Qingyun Liu,Yukou Du
Mastery over the structure at nanoscale can efficiently tune the catalytic properties of catalysts, enabling great enhancement in electrocatalytic performance toward liquid fuel electrooxidation reactions. Herein, we demonstrate a facile one-pot method for the successful fabrication of binary PdCu nanocatalysts bounded with 3D open-structured nanocages , which show the advantages of high surface areas, facile mass/electron transport, and strong synergistic effect. Impressively, the resultant 3D open-structured PdCu nanocages (NCs) show large promotion in electrocatalytic performance toward ethanol oxidation reaction (EOR) with the mass activity of 1790.8 mA mg −1 , being 3.3 times higher than that of commercial Pd/C (536.2 mA mg −1 ). Besides, the specific activity for EOR on PdCu NCs (7.7 mA cm −2 ) is also comparable to many Pt-based electrocatalysts , suggesting the dramatically improved electrocatalytic activity . The outstanding electrocatalytic performance of binary PdCu catalysts is attributed to the highly open 3D nanocage structure and strong electronic effect of Pd and Cu.
研究领域:
材料科学
·
电化学
·
催化领域
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Shang-Xiong Wei,Yu-Hang Yang,Xue-Bo Liu,Xiao-Bin Ye,Xiao-Peng Zhao,Xue-Wei Pi,Xue-Feng Cheng,Jing-Hui He
The electrochemical reduction reaction of nitrate (NO 3 RR) to ammonia is an environmentally friendly approach that can treat wastewater as well as find an alternative to the energy-intensive Haber-Bosch process. The use of adhesives partially to adhere to the NO 3 RR electrocatalysts, leading to sluggish kinetics, poor stability and poor scalability. Herein, we report the synthesis of PdCu alloy catalysts via a direct laser writing method, demonstrating their exceptional performance in the electrochemical reduction of nitrate. The Pd 0.55 Cu 0.45 alloy exhibited a remarkable ammonia production rate of 30.55 mg h −1 cm −2 under neutral electrolyte conditions and maintained stable operation for over 1500 h. Density functional theory (DFT) calculations and experimental analyses revealed that the PdCu alloy’s enhanced activity stems from its lower energy barrier for the rate-determining step (*NO → *NOH) and improved mass transfer capabilities. The alloy’s electronic properties and geometric configuration, fine-tuned by the laser-induced synthesis method, facilitate the conversion of NO 2 − and suppress the hydrogen evolution reaction (HER), thereby significantly enhancing the selectivity and activity of the NO 3 RR process. This study provides a sustainable and efficient pathway for ammonia synthesis and offers insights into the design of advanced catalysts for environmental and energy applications.
研究领域:
环境科学
·
电催化
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Jianfeng Li,Wenli Suo,Yuena Huang,Minglin Chen,Haowen Ma,Chuang Liu,Huan Zhang,Kun Liang,Zhengping Dong
The selective hydrogenation of alkynes to alkenes is widely applied in the chemical industry; nevertheless, achieving highly selective hydrogenation with high catalytic activity is considerably challenging. Herein, ultrafine PdCu bimetallic nanoparticles encapsulated by high-surface-area mesoporous α-Al 2 O 3 were prepared by high-temperature calcination–reduction using a porous organic framework (POF) as the template. As-obtained PdCu@α-Al 2 O 3 exhibited a high selectivity of 95% for the semi-hydrogenation of phenylacetylene as a probe reaction under mild reaction conditions. The separation of continuous Pd atoms and modification of the Pd electronic state by Cu atoms suppressed β-hydride formation and alkene adsorption, contributing to high selectivity for the catalytic hydrogenation of alkynes. The catalytic activity was maintained after 7 cycles due to the strong interaction between the PdCu bimetallic nanoparticles and α-Al 2 O 3 as well as the encapsulation effect of mesoporous α-Al 2 O 3 . Thus, the current work provides a facile strategy for fabricating high-surface-area mesoporous α-Al 2 O 3 -supported catalysts for industrial catalysis applications.
研究领域:
化学工程
·
材料科学
·
催化反应
✓ 已验证
DOI
PubMed
高影响因子
ChemistrySelect
·
2024
·Vol. 9
·期 31
·e202400459
·
IF 1.9
Yongyu Huang,Xinxin Xia,Pei Li,Yaqian Gu,Hua Song,Cuiqin Li,Feng Li
Graphical Hydrogenation of furfural to furfuryl alcohol under H 2 and N 2 atmosphere are studied over PdCu/ZrPO with metal and Lewis acid sites. The PdCu metal active sites of PdCu/ZrPO involve both direct hydrogenation and transfer hydrogenation activities, and the Zr 4+ −O 2− Lewis acid-basic pairs of ZrPO have transfer hydrogenation activity. Hydrogenation of furfural to furfuryl alcohol under H 2 and N 2 atmosphere was studied over zirconium phosphonate (ZrPO)-supported PdCu (PdCu/ZrPO) catalysts. The direct hydrogenation and transfer hydrogenation activities of PdCu metal active sites and the transfer hydrogenation activity of Zr 4+ −O 2− Lewis acid-basic sites were investigated, respectively. The size and the distribution of Cu particles could be adjusted by altering the P/Zr molar ratio. Bimetallic PdCu could enhance the acidity of the PdCu/ZrPO catalysts, and improve the ratio of Lewis/Brønsted acid, which led to an increase in the transfer hydrogenation activity of Lewis acid-basic pairs. The electronic effect between Pd and Cu promoted furfural to absorb onto electron-deficient Cu through η1(O)-aldehyde configuration, which contributed to the direct hydrogenation and the transfer hydrogenation at metal active sites. Especially, the adsorption and dissociation of H 2 in electron-rich Pd were promoted, which significantly improved the direct hydrogenation activity.
研究领域:
催化化学
·
能源化学
✓ 已验证
DOI
高影响因子
ChemNanoMat
·
2026
·Vol. 12
·期 1
·e202500682
·
IF 2.6
Jingzhou Liu,Yangjun Guo,Xiaojun Zeng
Direct ethanol fuel cells have attracted significant attention due to their high energy density, environmental friendliness, fuel availability, and low toxicity. However, their broader application is constrained by the anode catalyst limitations such as low active site density and low stability caused by the CO* intermediate poisoning. In this work, Pd metallene was synthesized via a hydrothermal method, and transition metal Cu was introduced to obtain PdCu bimetallene supported with porous Cu nanoparticles (NPs). The results indicate that the unique configuration of Cu not only enhances the CO* intermediate tolerance of Pd through electronic interactions but also leverages the intrinsic catalytic activity of Cu, leading to a further improvement in catalytic performance. Therefore, the designed PdCu bimetallene/Cu NPs exhibits a high mass activity of 1.26 A mg Pd −1 for the ethanol electro oxidation reaction, which is 8.4 times that of commercial Pd/C and superior to recently reported Pd-based catalysts. In addition, it maintains a current density of 7.87 mA cm −2 after a 3000 s stability test, demonstrating considerable potential for practical applications. This work provides feasible ideas for the microstructure design and electronic control optimization of metallene in small molecule catalysis.
✓ 已验证
DOI
高影响因子
Catalysts
·
2025
·Vol. 15
·期 7
·610
·
IF 4
Wei Wang,Jiaqi Liu,Guang Shi,Shiqi Wu,Nan Zhang,Ruixia Yuan
Spherical Cu2O nanoparticles were obtained by reducing copper acetate in N,N-dimethylformamide (DMF) system using glucose as the reducing agent and polyvinylpyrrolidone (PVP) as the surfactant, with which spherical PdCu nanocatalysts were thus synthesized by disproportionation. The catalyst was used for the activation of peroxymonosulfate (PMS) and showed an excellent degradation effect on rhodamine B and methylene blue-contained printing and dyeing wastewater with good stability. Additionally, the surface morphology analysis of the catalyst was carried out by SEM and TEM. The structure was characterized by XRD and FT-IR. The valence state and composition of the catalyst were characterized by XPS. The catalytic performance of the prepared catalysts was investigated with methylene blue and rhodamine B used as target pollutants. The results showed that the catalytic reduction efficiency of PdCu nanocatalyst for the two pollutants could reach 99% at 20 °C, when catalyst concentration was 60 mg/L and PMS concentration was 1.0 g/L and 0.6 g/L, respectively. The degradation efficiency of the catalyst was significantly reduced when Cl−,HCO3−and HA were present in the water. The degradation efficiency was above 90% when the pH was in the range of 5–11. The excellent performance of the PdCu/PMS system in the treatment of RhB-contained wastewater was further confirmed by taking into account of the data of free radical quenching experiment and the results of electron paramagnetic resonance (EPR) experiment. After three cycles, the removal rate of MB and RhB could still be maintained at more than 90%, which proved its excellent recyclability due to its remarkable stability and efficiency.
✓ 已验证
产品关联
DOI
高影响因子
Journal of Physical Chemistry C
·
2025
·
IF 3.2
Qiuchen Yang,Yamei Xu,Ziluo Ding,Ruijun Hou
PdCu bimetallic catalysts can enhance both selectivity and activity simultaneously in the selective hydrogenation of 1,3-butadiene, although the mechanism behind the enhanced performance of the PdCu catalysts remains insufficiently understood. The presence of mixed and disordered alloy phases on the bimetallic catalyst surface hinders the identification of the intrinsic reaction mechanism. In the current work, catalysts with well-defined Pd, Pd1Cu1, Pd1Cu3 alloy phases were controllably synthesized to investigate the selective hydrogenation performance of 1,3-butadiene. It is found that Pd1Cu1/SiO2 and Pd1Cu3/SiO2 exhibit not only higher intrinsic activity but also higher selectivity toward total butenes and 1-butene than Pd/SiO2 due to the electronic effect, which becomes more significant with increasing Cu/Pd. Furthermore, ideal Pd(111), Pd1Cu1(111), and Pd1Cu3(111) surfaces were modeled by DFT calculations to conduct theoretical studies. It is found that the electronic effect is more significant and the adsorption energy to butenes decreases with increasing Cu/Pd ratio. By analyzing the transition states of the elementary reactions in the reaction pathways, the reaction mechanisms are revealed on different surface sites. It is indicated that the bimetallic PdCu surfaces exhibit higher intrinsic hydrogenation activity and higher selectivity to total butene and 1-butene, in agreement with the experimental results.
研究领域:
催化化学
·
材料化学
·
表面科学
·
理论化学
·
纳米催化
·
能源化学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Jiabing Geng,Yafang Luo,Jiale Song,Hongjie Yu,You Xu,Hongjing Wang,Kai Deng,Ziqiang Wang,Liang Wang
Electrocatalytic reforming of polyethylene terephthalate (PET)-derived ethylene glycol (EG) into high-value glycolic acid (GA) is a potential strategy for PET plastic upcycling, and the efficiency mainly depends on the identification of high-performance electrocatalysts. In this study, we synthesize Ga-incorporated PdCu metallene (GaO x -PdCuene) with an oxygen-bridge structure (GaO x -PdCuene) for the electrolysis of PET hydrolysate towards GA production. GaO x -PdCuene demonstrates an impressive Faradaic efficiency of 98.72 % for GA production at a potential of 0.9 V, along with stable operation for over 100 h. The experimental and theoretical analyses show that the Ga-induced oxygen-bridge structure, accompanying with p-d orbital hybridization, efficiently regulates electronic structure of Pd, which effectively facilitates *OH species generation and optimizes adsorption energies of intermediates on Pd active sites, leading to high activity and selectivity for GA generation. The work highlights the design of oxygen-bridge structure in Pd-based electrocatalysts for efficient conversion of PET wastes to high-value GA product.
研究领域:
材料化学
·
环境催化
·
可持续能源
·
高分子化学
·
电化学
·
纳米材料
·
绿色化学
✓ 已验证
产品关联
DOI
高影响因子
TURKISH JOURNAL OF CHEMISTRY
·
2023
·Vol. 47
·期 1
·207-217
·
IF 1.4
JİANG ZHIJIE,FU SHUIYUAN,ZHAO WEI,LIU XVTANG,WANG FEI,CUI MINGYU,DONG LINYANG
Fabricating highly efficient Pd-based nanocatalysts with a well-defined structure is desired for the commercialization of direct ethanol fuel cell (DEFC). Herein, a series of hierarchical three-dimensional N-doped hollow graphene spheres (NHGS) supported dendritic PdCu alloy catalysts Pd$_{x}$Cu$_{(d)}$-NHGS (x: Cu/Pd theoretical molar ratio of 4, 2, and 1) are assembled by one-pot ascorbic acid reduction-immobilization method. Aiming to maximize the Pd utilization and realize the efficient ethanol electrooxidation, this novel electrocatalyst offers potent activity sites and promotes electron and ion kinetics simultaneously. Characterization indicates that the as-obtained Pd$_{4}$Cu$_{(d)}$ alloy nanoparticles with average sizes of approximately 55 nm are evenly dispersed on the NHGS supporting materials obtained by using the SiO2 nanospheres template strategy. Three catalysts all exhibit enhanced electrocatalytic activity, of which the Pd$_{4}$Cu$_{(d)}$-NHGS shows the highest mass current activity (2683 mA mg$_{Pd}$$^{-1}$), which is 2.59 times of the commercial Pd/C toward ethanol electrooxidation in alkaline medium. Based on the results, we believed that the Pd$_{4}$Cu$_{(d)}$-NHGS could exhibit extensive application prospect in alkaline DEFC. Key words:
✓ 已验证
DOI
高影响因子
ACS Applied Energy Materials
·
2018
·
IF 0
Shao-Qing Liu,Yi-Tao Xu,Jin-Qi Xie,Guo-Qing Sheng,Yan-Wu Zhu,Xian-Zhu Fu,Rong Sun,Ching-Ping Wong
Novel bowl-like, apple-like, and spherical PdCu alloy hollow microparticles with mesoporous nanoshells are synthesized through a simple disproportionation reaction route using a spherical Cu2O template with increasing H2PdCl4 ratio. The diameter of hollow particles is about 1 μm, and the thickness of mesoporous shells is about 50 nm. The obtained bowl-like PdCu alloy hollow microparticles with mesoporous nanoshells exhibit the highest electrocatalytic activity among the apple-like and spherical PdCu hollow microparticles and commercial Pd/C electrocatalysts toward methanol anodic oxidation for fuel cells. The remarkably excellent electrocatalytic performance of bowl-like PdCu alloy electrocatalysts might be attributed to the unique bowl-like hollow architecture with highly mesoporous nanoshells which are constructed by self-supported PdCu nanoparticles. The strategy presented here might help pave the way for the synthesis of novel nano-/microcomplex hollow materials with mesoporous nanoshells.
研究领域:
材料科学
·
电化学
·
纳米技术
✓ 已验证
DOI
危险品化学品经营许可证（带存储）