INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2018
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IF 4.229
Ying-Hua Zhou,Zhiyan Zhang,Suqin Wang,Nicholas Williams,Yong Cheng,Shizhong Luo,Jing Gu
The hydrogen economy is a proposed system that utilizes hydrogen to deliver energy. For the realization of this concept, how to safely, controllably and reversibly store and release hydrogen are critical problems which must be resolved. Metal alloys combined with suitable support materials are widely applied to various catalytic reactions . Here palladium nickel bimetallic nanoparticles doped with cerium oxide on a reduced graphene oxide (rGO) support were prepared by combining metal ion precursors and graphene oxide in a one-pot co-reduction approach. The as-received catalysts were characterized by XRD , TEM, SEM, XPS and ICP-OES, and the results revealed that PdNi-CeO 2 nanoparticles were uniform dispersal on rGO. The as-synthesized PdNi-CeO 2 /rGO had been adopted as a heterogeneous catalyst for the hydrogen evolution from the hydrolysis of ammonia borane (NH 3 BH 3 , AB) at room temperature . Kinetically, the hydrogen-release rate was first-order with the increased concentration of catalysts. The optimized catalyst of Pd 0.8 Ni 0.2 -CeO 2 /rGO with the CeO 2 content of 13.9 mol% exhibited an excellent activity with a turnover frequency value of 30.5 mol H 2 (mol catalyst) −1 min −1 at 298 K, and a low apparent activation energy ( E a ) of 37.78 kJ mol −1 . The robust catalytic performance of the Pd 0.8 Ni 0.2 -CeO 2 /rGO is attributed to the uniform controlled nanoparticle size, the synergic effect between the nanoparticles bimetallic properties, and the effective charge transfer interactions between the metal and support.
研究领域:
催化化学
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材料科学
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DOI
高影响因子
Molecular Catalysis
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2022
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IF 5.089
Jianfeng Li,Jinfang Kou,Yongsheng Xiang,Minglin Chen,Junyi Zhang,Xuecheng Zhan,Huan Zhang,Fushan Wang,Zhengping Dong
Catalytic semi-hydrogenation of alkynes to alkenes plays an important role in the polymer, fragrance, medicine, and other chemical industrial fields. However, increasing the selectivity of alkenes during the semi-hydrogenation process is a huge challenge. Herein, N-doped porous carbon support (NC) was fabricated from zinc-based zeolite imidazole frameworks (ZIF-8). Ultrafine PdNi bimetallic nanoparticles (NPs) were uniformly dispersed, stably anchored on the NC support, and used as an efficient alkynes semi-hydrogenation catalyst. The synthesized Pd 2 Ni 2 /NC catalyst had a selectivity of 95.1% toward styrene and high catalytic activity (TOF=977.7 h −1 ) for the semi-hydrogenation of phenylacetylene under mild reaction conditions. The catalyst was mainly through metal-support interaction and electron transfer between Pd and Ni metal, modulating the electronic structure of the active sites, thus improving the selectivity of styrene. Selective hydrogenation of various substituted alkynes on Pd 2 Ni 2 /NC catalyst has also proved excellent applicability, and the obtained catalyst can be reused with favorable stability. This study adjusted the catalytic performance by adding a secondary metal, which provided a useful strategy for designing highly efficient catalysts for the semi-hydrogenation of alkynes.
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高影响因子
CATALYSIS TODAY
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2023
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IF 5.3
Yue Hua,Jingsen Zhang,Tengda Zhang,Aimin Zhu,Guangqing Xia,Xiuling Zhang,Lanbo Di
Catalytic removal of 4-nitrophenol (4-NP) in wastewater remains a significant challenge due to the poor activity and stability of the catalysts. Herein, low-cost graphite oxide (GO) supported Pd and Ni NPs (PdNi/GO) with enhanced catalytic activity and stability for 4-NP reduction were synthesized by a plasma method in the aqueous solution of Pd(NO 3 ) 2 , Ni(NO 3 ) 2 , and GO. The normalized rate constant k nor over the PdNi/GO with Pd/Ni= 1.8:0.2 for 4-NP reduction was as high as 5480 min −1 ·g −1 ·L, which was comparable with that of Pd/GO, and it was about 50.7 times higher than that of Pd/rGO-H prepared by traditional thermal reduction method. Importantly, after six reaction cycles, it only decreased to 74.8% of the initial value, which was much higher than that of the Pd/GO catalyst (59.8%). The characterization results indicated that plasma synthesized Pd/GO catalyst can keep the oxygen-containing groups (OCGs) on the GO surface , generate abundant defects, and facilitate the adsorption of the 4-NP. Interestingly, the addition of Ni could keep these merits, and the formed PdNi alloyed structure may facilitate the electron transfer between PdNi NPs and GO, contribute to the strong adsorption of 4-NP and the rapid generation of active hydrogen. Consequently, the PdNi/GO catalyst exhibited outstanding catalytic activity and stability for 4-NP reduction. This work provided a fast, facile, environmentally friendly, and easy to scale up plasma method for synthesizing high performance Pd-based catalysts.
研究领域:
环境催化
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纳米材料
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物理化学
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水处理
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能源与环境科学
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DOI
高影响因子
ACS Applied Nano Materials
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2024
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IF 5.3
Qingqing Liu,Xin Deng,Lihua Zhu,Ping Huang,Weizhen Wang,Liqing Li,Zhiqing Yang,Huan Zhang,Junyuan Xu,Hengqiang Ye
To obtain a recyclable and environmentally friendly solid catalyst with excellent catalytic properties and selectivity for 4-nitrophenol (4-NP) hydrogenation, herein, covalent organic frameworks (COFs) are used as the support. Tiny PdCo alloy particles are confined in the pores of the COFs to acquire PdCo/COFs, with an extremely narrow PtCo size distribution (6.28 ± 2.85 nm). The effect of Pd+Co loading and the Pd/Co atomic ratio on the catalytic behaviors of PdCo/COFs for 4-NP hydrogenation is explored. The as-gained PdCo/COFs catalyst (Pd─1.72, Co─1.23 wt %) exhibits good catalytic behaviors (conversion─90.5%, selectivity to 4-aminophenol (4-AP) > 99.0%, and conversion─11.0%, selectivity to 4-aminophenol (4-AP) > 99.0%, TOF─turnover frequency─44.2 min–1) for 4-NP hydrogenation under quite moderate reaction conditions (40 °C, 3.0 MPa hydrogen pressure), and PdCo/COFs have superior stability. Additionally, the catalytic property of PdCo/COFs is better than that of monometallic supported catalysts (Pd/COFs or Co/COFs) and PdNi/COFs. It can be considered that the formation of the PdCo alloy particles is beneficial to the activation of 4-NP. The PdCo/COFs catalysts are analyzed by XRD, XPS, ICP-OES, SEM-EDX, BET, TEM, HRTEM, STEM-EDX elemental analysis, and aberration-corrected STEM (AC-STEM), confirming that tiny PdCo alloy particles are uniformly loaded on the COFs. The PdCo/COFs samples have the advantages of outstanding stability and thus their own desired industrial application potential.
研究领域:
材料科学
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催化化学
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DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
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2026
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IF 6.7
Lan Zhang,Wanran Huang,Xi Peng,Peixin Jiang,Jianshan Ye,Minglei Yan,Zhiwei Lu
The high efficiency, low cost, and rapid preparation of non-noble metal oxygen reduction reaction (ORR) electrocatalysts are of great significance for the large-scale application of energy conversion equipment. Herein, PdNi alloy nanoparticles dispersed within the multiwalled carbon nanotubes (MWCNTs) composite (PdNi-PVP/MWCNTs) were synthesized via an in situ self-assembly strategy, in which polyvinylpyrrolidone (PVP) serves as an N and C source, and MWCNTs act as conducting supports to enhance structural integrity and electron transport. Notably, the synthesis relies solely on low-temperature oil-bath stirring, enabling rapid batch production without the need for high-temperature calcination-a distinctly green and scalable approach. In this system, PVP acts as a capping agent that facilitates the uniform anchoring of PdNi alloy nanoparticles on MWCNTs, effectively suppressing particle aggregation, thereby increasing the surface roughness and specific surface area to expose more active sites. Impressively, benefiting from the unique structure, high crosslinking, and high conductivity that minimize catalyst separation and aggregation, this new type of electrocatalyst exhibited an impressive ORR onset potential of 0.97 V, half-wave potential of 0.83 V, larger current density of 4.3 mA∙cm −2 , and existing good corrosion resistance to drive a relatively stable performance, which are superior to commercial Pt/C in alkaline media. This study demonstrates the successful design of an environmentally benign and cost-effective ORR electrocatalyst, highlighting its promising potential for practical applications in energy conversion technologies.
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高影响因子
ACS Catalysis
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2016
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IF 9.307
Qiaofei Zhang,Xin-Ping Wu,Yakun Li,Ruijuan Chai,Guofeng Zhao,Chunzheng Wang,Xue-Qing Gong,Ye Liu,Yong Lu
A Ni-foam-structured PdNi nanoalloy catalyst engineered from nano- to macro-scales has been successfully fabricated for the catalytic deoxygenation of coalbed methane (CBM). The catalyst was obtainable by embedment of Pd nanoparticles onto Ni-foam substrate via a galvanic exchange reaction method and subsequent in situ activation in the reaction, which was active at low temperature, selective (no CO formation), and oscillation free in this CH4-rich catalytic combustion process. Special Pd@NiO (Pd nanoparticles partially wrapped by tiny NiO fragments) ensembles were formed in the galvanic deposition stage and could merely be transformed into PdNi nanoalloys in the real reaction stream at elevated temperatures (e.g., 450 °C or higher). Density functional theory (DFT) calculations were carried out to reveal the role of Ni decoration at Pd in PdNi nanoalloy catalyst for the CBM deoxygenation. By nature, the Pd–Ni alloying modified the electronic structure of surface Pd and led to a decrease in the O adsorption energy, which can be taken as the activity descriptor for the CBM deoxygenation. A reaction kinetic study indicated that the Ni decoration at Pd by Pd–Ni alloying lowered the apparent activation energy in comparison to the pristine Pd catalyst, while leading to an increase of the reaction order of O2 from −0.6 at Pd catalyst to −0.3. The foam-structured PdNi nanoalloy catalyst thus offered enhanced low-temperature activity and the elimination of oscillating phenomena as the result of a transient balance obtained between the cycles of O2 adsorption/activation and CH4 oxidation.
研究领域:
催化化学
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材料科学
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能源工程
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计算化学
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环境化学
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DOI
高影响因子
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