MICROPOROUS AND MESOPOROUS MATERIALS
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2024
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IF 4.8
Hongyan Wang,Xinyue Sun,Jingpei Cao,Yajie Tian,Bofeng Zhang
Zeolite catalysts have been widely applied in petroleum and chemical industries. Nano/hierarchical structure could improve the utilization efficiency of active sites, especially for metal species encapsulated in zeolites. However, the uniformity of zeolite surface and crystallinity would decrease, leading to low stabilization effect. Herein, we developed a seed-directed method to prepare Pd clusters (∼1.3 nm) regioselectively encapsulated in hollow polycrystalline shell of Silicalite-1 zeolite. In nitrobenzene hydrogenation reaction, the optimized Pd@S-1-hp showed a high conversion of 92.2 % at 110 °C, which is 40 % higher than that of Pd clusters in bulk zeolite. Sub-nano Pd species in polycrystalline shell could significantly shorten the diffusion length on the basis of strong microporous confinement effect. Catalytic hydrogenation activity remained stable after six cycles. This structure could be extended to heterogeneous reactions suffering from diffusion limitation.
研究领域:
化学工程
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催化材料
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ACS Applied Materials & Interfaces
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2021
·
IF 9.229
Yu-Chuan Jiang,Hui-Ying Sun,Ya-Nan Li,Jia-Wei He,Qi Xue,Xinlong Tian,Fu-min Li,Shi-Bin Yin,Dong-Sheng Li,Yu Chen
Methanol electrolysis is a promising strategy to achieve energy-saving and efficient electrochemical hydrogen (H2) production. In this system, the advanced electrocatalysts with high catalytic performance for both the methanol oxidation reaction (MOR) and hydrogen evolution reaction (HER) are highly desirable. Inspired by the complementary catalytic properties of rhodium (Rh) and palladium (Pd) for MOR and HER, herein, several Pd core–RhPd alloy shell nanodendrites (Pd@RhPd NDs) are synthesized through the galvanic replacement reaction between Pd nanodendrites (Pd NDs) and rhodium trichloride. For MOR, Pd@RhPd NDs exhibit Rh content-determined catalytic activity, in which Pd@Rh0.07Pd NDs have an optimal combination of oxidation potential and oxidation current due to the synergistic catalytic process of Pd/Rh double active sites. For HER, the introduction of Rh greatly improves the catalytic activity of Pd@RhPd NDs compared to that of Pd NDs, suggesting that Rh is the main activity site for HER. Unlike MOR, however, the HER activity of Pd@RhPd NDs is not sensitive to the Rh content. Using Pd@Rh0.07Pd NDs as robust bifunctional electrocatalysts, the as-constructed two-electrode methanol electrolysis cell shows a much lower voltage (0.813 V) than that of water electrolysis (1.672 V) to achieve electrochemical H2 production at 10 mA cm–2, demonstrating the application prospect of methanol electrolysis for H2 production.
研究领域:
材料科学
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电化学
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能源科学
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CHINESE JOURNAL OF CHEMICAL ENGINEERING
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2026
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IF 3.5
Hongda Zhang,Jinyan Hu,Shuting Bao,Shichao Su,Weiyao Yang,Le Sang
Designing efficient catalysts and solvent system for the multiphase hydrogenation reaction is vital in continuous flow reactors. Herein, we prepare hydrophilic Pd/Al 2 O 3 and hydrophobic modified C 12 PA-Pd/Al 2 O 3 catalyst for nitrobenzene (NB) hydrogenation in micropacked bed reactors (μPBRs). By tuning the methanol-water volume ratio, reaction temperature, reaction pressure, liquid and gas superficial velocity, the NB conversion and aniline (AN) yield are optimized. The highest NB conversion of 97.1% and AN yield 95.6% are obtained in μPBRs with hydrophobic C 12 PA-Pd/Al 2 O 3 at the reaction temperature of 90 °C. The apparent kinetic model is developed in μPBRs with two types of catalysts, and activity energies of NB hydrogenation for Pd/Al 2 O 3 and C 12 PA-Pd/Al 2 O 3 are 7.944 kJ·mol -1 and 3.372 kJ·mol -1 , respectively. It indicates that the catalytic efficiency of C 12 PA-Pd/Al 2 O 3 is better than that of Pd/Al 2 O 3 in the methanol-water mixed solvent in μPBRs. The value of TOF for the hydrophobic modified C 12 PA-Pd/Al 2 O 3 catalyst is twice compared with the hydrophilic Pd/Al 2 O 3 catalyst. The value of STY for μPBRs is higher than that of stirred tank reactors (STRs) and fixed bed reactors (FBRs).
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INORGANIC CHEMISTRY
·
2023
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IF 4.6
Ziqiang Wang,Shan Xu,Qiqi Mao,Kai Deng,You Xu,Hongjing Wang,Hongjie Yu,Liang Wang
Designing two-dimensional (2D) materials functionalized with organic molecules is an effective tactic to enhance catalytic performances for the oxygen reduction reaction (ORR). Herein, we synthesize Pd metallene with in situ modification of polyethylenimine-ethylenediamine (Pd@PEI-EDA metallene), in which PEI-EDA serves as both the structure-directing agent and modifier. Pd@PEI-EDA metallene has ample active sites and tuneable electronic structures due to ultrathin nanosheets with abundant wrinkles and interfacial structure. In contrast with commercial Pd/C and Pt/C, Pd@PEI-EDA metallene displays preferable catalytic ORR performance under alkaline conditions. This work offers an in situ interface engineering tactic for the preparation of 2D polymer-metal electrocatalysts to boost the ORR performance.
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CHINESE JOURNAL OF CHEMICAL ENGINEERING
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2023
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IF 3.8
Qinqin Yuan,Jingyue Liang,Wei Li,Jinli Zhang,Cuili Guo
Anthraquinone hydrogenation to produce H 2 O 2 is an economically interesting reaction with great industrial importance. Here, we report a series of Pd/ x Al catalysts with different AlCl 3 contents by a conventional stepwise impregnation method. The optimal Pd/1.0Al catalyst exhibits a higher performance toward anthraquinone hydrogenation with 8.3 g·L −1 hydrogenation efficiency, 99.5% selectivity and good stability, obviously superior to that of Pd/Al 2 O 3 catalyst (5.2 g·L −1 and 97.2%). Detailed characterization demonstrates that AlCl 3 can be grafted on the γ-Al 2 O 3 support to obtain a modified support with abundant surface weak acid and Lewis acid, which can adsorb and activate anthraquinone. Meanwhile, its steric hindrance could isolate and disperse active metals to form more active sites. The synergies between metal sites and acid sites promotes the anthraquinone hydrogenation. Furthermore, the good stability after grafting AlCl 3 could attribute to the enhanced metal-support interaction inhibiting metal particles agglomeration and leaching.
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NANOTECHNOLOGY
·
2023
·Vol. 34
·期 35
·355402
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IF 3.5
Qian Liu,Seng Dong,Yuanzhe Wang,Weiyi Jia,Xi Chen,Faming Gao,Yatao Wang
Fuel cells, as the alternative to fossil energy, have engaged widespread attention by reason of the high conversion efficiency from the chemical energy to the electric energy combined with low pollution emissions. The cathodic ORR catalysts with excellent performance and cost-effectiveness are the dominant point towards the massive development of fuel cells. Here, our group select the Pd NWs as the template and construct the Pd@PtRuNi core–shell bilayer nanostructure to expand platinum atom utilization. Pd@PtRuNi bilayer core–shell NWs unfold elevated mass activity of 1.62\,{\rm{A}}\,{{\rm{mg}}}_{{\rm{metal}}}^{-1} at 0.9 V versus RHE in alkaline media, 2.03- and 6.23-fold of pristine Pd NWs and benchmark commercial Pt/C, respectively. Meanwhile, the cyclic stability tests reveal the excellent durability of Pd@PtRuNi NWs, whose mass activity is only 13.58% degradation after accelerated durability tests. The catalytic activity and durability towards ORR are better than the U.S. 2025 DOE target (0.44\,{\rm{A}}\,{{\rm{mg}}}_{{\rm{pt}}}^{-1} and less than 40% activity attenuation at 0.9 V after 30 000 potential cycles). The elevated catalytic properties can be traceable to the synergism between the ligand effect of Ni and Ru and one-dimensional structure superiority, which optimizes the electronic structure of active sites, promotes the charge transfer and restrains the agglomeration and detachment.
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ACS Applied Nano Materials
·
2022
·
IF 6.14
Haiyan Ruan,Shaofang Zhang,Hongguang Wang,Jiahui Pei,Ruoli Zhao,Xiaoyu Mu,Hao Wang,Xiaodong Zhang
The construction of nanozymes at the atomic level that hold structural stability and high enzyme-like activity is now a key factor in the optimization of an artificial enzyme. Single-atom metal/cerium oxide (CeO2)-based nanozymes have been demonstrated to possess a variety of enzymatic activities and radical scavenging abilities, which are mainly attributed to the single-atom active site, redox valence states, and abundant defect chemistry. Here, we developed a single-atom Pd/CeO2 nanostructure by aqueous phase synthesis that exhibits the advantages of high yield and good stability. The Pd/CeO2 nanostructure possesses peroxidase (POD), superoxide dismutase (SOD), and catalase (CAT) activities as well as reactive nitrogen species free-radical scavenging activity, exhibiting multienzyme-like activities and stability compared with CeO2 and other metal-based nanozymes. It is worth mentioning that the Pd/CeO2 nanostructure exhibits high POD-mimicking activity with a reaction rate of 0.88 μM/min, about 5 times higher than that of the CeO2 nanozyme. In addition, the CAT-like activity of the Pd/CeO2 nanostructure is excellent, and its scavenging rate of hydrogen peroxide reached nearly 100% at a concentration of 50 ng/μL. The present work shows that single-atom Pd substitution is a promising strategy for the design of CeO2 nanozymes to exert better effects on biomedical applications, especially with diseases related to oxidative stress.
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Journal of Environmental Chemical Engineering
·
2021
·
IF 5.909
Guanfeng Tian,Youqing Wu,Shiyong Wu,Sheng Huang,Jinsheng Gao
Synthesizing methanol from CO 2 and green hydrogen is a promising strategy to solve environmental issues and meet the increasing energy demand. In this work, Pd/MnO/In 2 O 3 catalyst with highly dispersed Pd species was prepared via an in-situ reduction method using NaBH 4 as the reducing agent. The highly dispersed Pd species promoted the dissociative of hydrogen and the hydride species could spill over to the MnO/In 2 O 3 due to the strong metal-support interaction between Pd and MnO/In 2 O 3 , which improved the catalytic activity of Pd/MnO/In 2 O 3 for CO 2 hydrogenation to methanol. As a result, the methanol space-time yield of 1 wt% Pd/MnO/In 2 O 3 was 4.8 times higher than that of MnO/In 2 O 3 . Moreover, the methanol selectivity of 1 wt% Pd/MnO/In 2 O 3 was still higher than 70% at a temperature below 280 °C. The present in-situ reduction method is an effective route for the preparation of Pd/MnO/In 2 O 3 catalyst for CO2 hydrogenation to methanol.
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BIOMATERIALS
·
2021
·
IF 12.479
Yunjian Yu,Jie Li,Boyi Song,Zhuang Ma,Yufei Zhang,Haonan Sun,Xiaosong Wei,Yayun Bai,Xueguang Lu,Peng Zhang,Xinge Zhang
Checkpoint inhibitors, such as antibodies blocking the PD-1/PD-L1 pathway, are among the most promising immunotherapies to treat metastatic cancers, but their response rate remains low. In addition, the usage of monoclonal antibodies as checkpoint inhibitors is associated with a series of drawbacks. Herein, an all synthetic nanoparticle with PD-L1 blockade capability is developed for cancer photothermal-immunotherapy. The polymeric nanoparticle integrates photothermal treatment, antitumor vaccination, and PD-1/PD-L1 blockade in a single system to augment the antitumor efficacy. In a CT26 bilateral tumor model, intravenously injected nanoparticles accumulate in tumor sites and mediate strong photothermal effects, eradicate the NIR treated primary tumors and elicit strong antitumor immunity by inducing immunogenic cell death (ICD). Growth of the untreated distant tumors is also suppressed due to the synergies of systemic antitumor immune activation and PD-L1 blockade. Our strategy offers a simple but promising approach for the treatment of metastatic cancer.
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JOURNAL OF CHEMICAL AND ENGINEERING DATA
·
2020
·
IF 2.369
Yongkang Lu,Bo Zhang,Shaobo Liu,Luxia Yin,Wanghui Gong,Jianguang Gao,Zekai Zhang,Wensheng Ning
Pd/SiO2-n aerogel composites with different Si/Pd mole ratios (n(Si/Pd)) were synthesized by a sol–gel method followed by drying in the atmosphere to adsorb thiophenic compounds from model oils. For Pd/SiO2-n, doping Pd species in SiO2 aerogels led to the appearance of weak Lewis acidic sites on the surface. The adsorption capacity of Pd/SiO2-n was significantly higher than that of pure SiO2, owing to the π-complexation, S–M bonding, and acid–base interaction between Pd2+ and thiophenic compounds. Among them, the capacity of Pd/SiO2-318 was the highest, 4.76 mg S/gads (i.e., 9.37 μmol S/μmol Pd), which was obviously higher than that of sorbents reported such as Pd/activated carbon and Pd/Al2O3, based on the amount of thiophene adsorbed per unit active centers. In the presence of aromatics and olefins, the selectivity of Pd/SiO2 for thiophene was higher than that of Ag/SiO2 and Cu/SiO2 reported, attributed to the stronger S–Pd bonding than the S–Ag and S–Cu bonding. The equilibrium adsorption data of thiophene onto Pd/SiO2-318 were well simulated with the Langmuir and Freundlich models. Combined with thermodynamic results, it can be found that the low temperature was favorable for the adsorption of thiophene. Pd/SiO2 exhibited a good regeneration performance after solvent washing.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2017
·
IF 3.133
Ke Zhang,Zhiping Xiong,Shumin Li,Bo Yan,Jin Wang,Yukou Du
Herein, we reduced PdCl 4 2− ions on the synthetized cuprous phosphide/reduced graphene oxidation (Cu 3 P/RGO) hybrids to improve the catalytic activity and durability of Pd nanocrystals . In comparison with commercial Pd/C and Pd/RGO catalysts, the Pd/Cu 3 P/RGO exhibit high electroactivity and durability toward alcohol oxidation in alkaline medium. The enhanced catalytic performance of Pd/Cu 3 P/RGO is due to the high electrochemically active surface area, which can be ascribed to the interactions between Cu 3 P/RGO and Pd nanocrystals . The investigation of Cu 3 P/RGO as a promoter in alcohol electrooxidation will offer an opportunity in the field of direct alcohol fuel cells (DAFCs).
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INORGANIC CHEMISTRY
·
2024
·
IF 4.3
Hugang Zhang,Guanghui Yang,Xinmiao Li,Yile Wang,Kai Deng,Hongjie Yu,Hongjing Wang,Ziqiang Wang,Liang Wang
Electrochemical conversion of nitrogen into ammonia at ambient conditions as a sustainable approach has gained significant attention, but it is still extremely challenging to simultaneously obtain a high faradaic efficiency (FE) and NH3 yield. In this work, the interstitial boron-doped porous Pd nanotubes (B–Pd PNTs) are constructed by combining the self-template reduction method with boron doping. Benefiting from distinctive one-dimensional porous nanotube architectonics and the incorporation of the interstitial B atoms, the resulting B–Pd PNTs exhibit high NH3 yield (18.36 μg h–1 mgcat.–1) and FE (21.95%) in neutral conditions, outperforming the Pd/PdO PNTs (10.4 μg h–1 mgcat.–1 and 8.47%). The present study provides an attractive method to enhance the efficiency of the electroreduction of nitrogen into ammonia by incorporating interstitial boron into porous Pd-based catalysts.
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