Nanoscale
·
2018
·Vol. 10
·期 47
·22348-22356
·
IF 7.233
Xusheng Cheng,Dongxu Wang,Jiancong Liu,Xin Kang,Haijing Yan,Aiping Wu,Ying Gu,Chungui Tian,Honggang Fu
Decreasing Pd usage whilst maintaining a superior performance is promising, but remains a challenge in the catalytic field. Herein, we have demonstrated the highly efficient promotion of Mo2N with a reduced amount of Pd for the liquid-phase hydrogenation reaction. The Mo2N (2–3 nm) was uniformly anchored onto mesoporous SBA-15 by using PMo12 as the Mo source. The small size and good dispersion of Mo2N is favourable for allowing their effective contact with post-loading Pd. This good contact is conducive to developing a synergistic catalyst, which was verified by studying the liquid-phase hydrogenation of p-nitrophenol (PNP) to p-aminophenol (PAP) with NaBH4 as the H source. The conversion ability of PNP to PAP on 1 wt% Pd–Mo2N/SBA-15 was vastly superior to 1 wt% Pd/SBA-15 and even better than 20 wt% Pd/SBA-15. The low-Pd, highly efficient catalysis is ascribed to the transfer of the electrons from Mo2N to Pd for the easy activation of H. The synergy can be affected by the type of support used. SBA-15 is superior to SiO2 and the other supports, which could be related to the large surface area and the plentiful number of pores on SBA-15, which is favourable to the dispersion of Pd and Mo2N, and the transfer/diffusion of the reactants. In particular, a highly efficient catalyst can be achieved at an even more reduced Pd loading (0.05 wt%). The current method describes the design of a highly efficient catalyst for the hydrogenation reaction using low amounts of noble metals.
研究领域:
催化化学
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF CHEMICAL PHYSICS
·
2023
·Vol. 159
·期 12
·
IF 4.4
Liu Huimin,Yuan Chenyi,Wu Shipeng,Sun Chao,Huang Zhen,Xu Hualong,Shen Wei
Surface property modification of catalyst support is a straightforward approach to optimize the performance of supported noble metal catalysts. In particular, oxygen vacancies and hydroxyl groups play significant roles in promoting noble metal dispersion on catalysts as well as catalytic stability. In this study, we developed a nanoflower-like TiO 2 -supported Pd catalyst that has a higher concentration of oxygen vacancies and surface hydroxyl groups compared to that of commercial anatase and P25 support. Notably, due to the distinctive structure of the nanoflower-like TiO 2 , our catalyst exhibited improved dispersion and stabilization of Pd species and the formation of abundant reactive oxygen species, thereby facilitating the activation of CO and O 2 molecules. As a result, the catalyst showed remarkable efficiency in catalyzing the low-temperature CO oxidation reaction with a complete CO conversion at 80 °C and stability for over 100 h.
研究领域:
催化化学
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED SURFACE SCIENCE
·
2025
·
IF 6.9
Yanan Wei,Tao Xia,Tongyu Zhong,Henghui Zhu,Yucai He,Yunlei Zhang
Interface engineering is a significance strategy to afford efficient selective oxidation for supported catalysts. Herein, constructing of frustrated Lewis pairs (FLPs) sites on CeO 2 and supporting Au-Pd nanoparticles to provide a highly selective production of 2,5-furandicarboxylic acid (FDCA) from 2,5-bis(hydroxymethyl)furan (BHMF). Mechanism investigations illustrate that the FLPs active sites enhance the adsorption and activation of catalyst for BHMF, decreasing the activation energy of rate-determining step. Simultaneously, the FLPs sites induce the electron transfer of the catalyst, generating a novel Au-Pd-CeO 2 interface that promotes the adsorption of molecule oxygen and the formation of the superoxide radical. Thereby, the Au x Pd y /P T -CeO 2 catalysts enable superior catalytic performance, achieving a satisfactory turnover frequency of 55.29 h −1 and a highly FDCA yield of 94.0 %. Such interfacial FLPs sites exhibit the great potentials for the selective oxidation of various unsaturated compounds.
研究领域:
化学工程
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催化科学
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产品关联
DOI
高影响因子
CATALYSIS LETTERS
·
2024
·
IF 2.3
Zhao Chunzhi,Mao Dongsen,Meng Tao,Guo Qiangsheng,Yu Jun
Owing to the intrinsic nature of the uniformed topologies and ultrasmall Zr 6 nodes of Zr-MOFs, herein, we employed Zr-MOFs (UiO-66 and UiO-67), as opposed to the support of traditional ZrO 2 , to prepare the Pd catalysts for toluene degradation. Compared with the catalysts of Pd/UiO-66 and Pd/ZrO 2 , Pd/UiO-67 catalyst boosted an excellence catalytic performance for toluene degradation, giving the lowest T 90% value of 235 °C with long-term stability. With the assisting of the cavity confinement of Zr-MOFs, Pd nanoparticles are prone to be encapsulated in the 3D frameworks of Zr-MOFs, and the bigger micropores of UiO-67 are more conducive to the formation of larger Pd nanoparticles. The in situ FT-IR results further declared that although the active sites are partly sacrificed due to the larger Pd nanoparticles formed in UiO-67, the stable adsorbed toluene on Pd/UiO-67 boosted the quick degradation of toluene in the reaction interval even without undergoing intermediate processes of benzoate and benzaldehyde. Graphical Abstract UiO-66, UiO-67 and ZrO 2 were employed to prepare the Pd catalysts for toluene degradation, Pd/UiO-67 catalyst boosted an excellence catalytic performance with long-term stability.
研究领域:
催化化学
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环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
Electrocatalysis
·
2014
·Vol. 6
·期 3
·255-262
·
IF 2.089
Lu Hai-Ting,Yang Zi-Juan,Yang Xin,Fan Yang
CeO 2 nanotubes with well-defined hollow interiors are employed as support material for Pd electrocatalysts towards formic acid oxidation (FAO). Pd nanoparticles are deposited both on the outer surfaces and inside interiors of CeO 2 nanotubes. The as-prepared Pd catalysts possess a large electrochemical surface area (ESA) and exhibit improved electrocatalytic performance towards FAO in comparison with the Vulcan XC-72 carbon black and the commercial CeO 2 powder supported Pd catalysts.
研究领域:
材料科学
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电化学
✓ 已验证
DOI
高影响因子
Frontiers in Chemistry
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2022
·
IF 5.545
Zhao Jinchong,Jiang Jie,Wen Song,Zhang Jing,Zhang Changsheng,Sheng Nan,Liang Wei,Sun Bing,Xu Wei,Yang Zhe,Pan Yuan
A series of alkali metal (Li, Na, and K)-modified Pd catalysts and Pd/Al2O3 were prepared and used to remove oxygen in a propylene flow with hydrogen’s existence. The results showed that the alkali metals could enhance the performance of the Pd catalysts and the effect followed the order of K > Na > Li. X-Ray diffraction (XRD), N2-physisorption, transmission electron microscopy (TEM), hydrogen temperature programmed reduction (H2-TPR), and X-ray photoelectron spectroscopy (XPS) were carried out to investigate the alkali metal-modified Pd catalysts and the promotional effect mechanism was explained. The results showed that alkali metal modification increased the electron density of Pd atoms to induce the negatively charged Pd species, which could enhance the adsorption of oxygen while weakening the adsorption of propylene, and then enhance the performance of the modified catalysts for oxygen removal from unsaturated hydrocarbon. The Pd-K/A catalyst performed the best on both oxygen removal and propylene hydrogenation inhibition.
研究领域:
催化化学
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材料科学
✓ 已验证
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2023
·
IF 4.7
Xin Song,Fangjun Shao,Zijiang Zhao,Xiaonian Li,Zhongzhe Wei,Jianguo Wang
Precise regulation of reaction selectivity at high conversions is the key to non-terminated alkyne semi-hydrogenation. Herein, a support modification strategy was employed to incorporate trace amounts of Mg elements into alumina support. The modified support loaded Pd catalyst optimized the activity and selectivity of the non-terminated alkyne semi-hydrogenation reaction. The TEM and XRD characterization of the catalysts demonstrated the entry of Mg elements into the Al 2 O 3 lattice to achieve the modification of the support. For the 2-butyne-1-ol semi-hydrogenation reaction, the Pd 0.5 /Mg 1 @Al 2 O 3 catalyst showed 99 % conversion and 97 % selectivity of the cis product at hydrogen pressure of 0.1 MPa and 25 °C. The introduced Mg element changed the electronic structure of Pd nanoparticles in the catalyst. The precise regulation of the 2-butyne-1-ol semi-hydrogenation reaction was achieved by adjusting the ratio of Pd 0 to Pd 2+ using the synergistic effect of Pd 0 and Pd 2+ .
研究领域:
催化化学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
AICHE JOURNAL
·
2023
·Vol. 69
·期 7
·e18078
·
IF 3.7
Yanping Yang,Jiarui Yang,Shucheng Shi,Yunhong Luo,Xingjun Xu,Yanan Liu,Dianqing Li,Junting Feng
Selective acetylene hydrogenation is a strongly exothermic process, easy to cause coking and metal agglomeration, and thus leads to deactivation. In this work, Pd/TiO 2 with different oxygen vacancies (V o ) were synthesized by controlling reduction temperature in 300–700°C, in which Pd/TiO 2 -HT300 (HT is reduction temperature) possessed the highest V o content. It was found highly dispersed Pd nanoparticles adjacent to more V o exhibited enhanced catalytic behavior (near 100% conversion at 55°C with 80% selectivity and turnover frequency of 0.12 s −1 ) due to hydrogen spillover generation and electron donation originating from V o sites, confirmed by in situ x-ray photoelectron spectroscopy, in situ Raman, and H 2 -temperature programmed desorption. More importantly, the increasing V o sites trap the released heat and devote to a decrease of heat accumulation over a single active Pd site, and consequently inhibit Pd agglomeration and polymerization, affirmed by high-resolution transmission electron microscopy, CO chemisorption, and thermogravimetric analysis.
研究领域:
催化化学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
NANOTECHNOLOGY
·
2023
·Vol. 34
·期 44
·445601
·
IF 3.5
Shuyuan Xu,Bingbao Mei,Fengjiao Li,Jianing Mao,Changxing Huang,Yufeng Yan,Ningning Chen,Yinghua Xu,Meiqin Shi
The application of electrochemical hydrodechlorination has been impeded due to the low utilization and activity of Pd catalyst. Herein, a series of Pd catalysts were prepared via the controllable evolution of Zn state during the pyrolysis of ZIF-8 nanosheet. Various forms of Pd with different chemical surroundings were generated upon the combined use of galvanic displacement and ion exchange process. Electrocatalytic hydrodechlorination of 4-chlorophenol was performed and the electrocatalytic hydrodechlorination efficiency of Pd/CN reaches 100% within 3 h at extra low Pd concentration. The coexistence of zero-valent Pd (Pd0) and nitrogen coordinated Pd (Pd–N) was verified by XAFS which provide multiple active sites for focusing on adsorbing H* and cracking C–Cl respectively. The synergetic effect between different chemical state of Pd for efficient hydrodechlorination of chloroaromatics and scheme for dexterous preparation of Pd based electrocatalyst are proposed and discussed.
研究领域:
环境科学
·
催化化学
✓ 已验证
DOI
高影响因子
APPLIED CATALYSIS A-GENERAL
·
2021
·
IF 5.706
Jiayu Song,Shengping Wang,Yan Xu,Qingling Liu,Yujun Zhao
Poor catalytic activity and stability are primary defects of traditional Pd/Al 2 O 3 catalysts for the low-temperature methane combustion. Herein, we developed a facile way to synthesize a MgAl-LDHs derived MgAl 2 O 4 spinel with good crystalline lattice and high surface area, which was used as support of Pd-based catalysts. Catalysts with Mg/Al ratio of 1/3 presented the highest methane combustion activity. It was found the well-crystallized MgAl 2 O 4 spinel promoted the dispersion and crystallization of PdO due to the strong interaction between PdO and support, and the electrophilicity and basicity originated from Mg doping suppressed the sintering of PdO particles, leading to the excellent performance of Pd/MgAl3. Moreover, these factors also inhibited the formation of surface OH- species, therefore, improved the water resistance. Such a synthesis strategy of the Pd/Mg x Al y derived from LDHs and the roles of MgAl 2 O 4 spinel could pose some meaningful directions for developing high-efficient Pd-based catalysts for the low-temperature methane combustion.
研究领域:
催化化学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF MATERIALS SCIENCE
·
2018
·Vol. 53
·期 21
·15064-15080
·
IF 2.993
Chen Jian,Ma Lei,Cheng Tingting,Cai Aofei,Hu Yuandong,Wu Zhijie,Liu Haiyan,Bao Xiaojun,Yuan Pei
In this work, a stable and recyclable Pd catalyst supported on N-containing silane coupling agent modified silica hollow microspheres with macroporous shells (Pd/N-SHMs) was successfully prepared and used for the selective hydrogenation of nitrile-butadiene rubber (NBR) with enhanced catalytic performance. The results showed that Pd/N-SHMs possessed small-sized and well-dispersed Pd nanoparticles (NPs) and the macroporous shells were beneficial for the diffusion of macromolecular NBR, and thus with such a catalyst, the reaction could occur under mild conditions and high hydrogenation degree (96.6%) with 100% selectivity to C=C was obtained. The prepared catalyst could be easily recycled and reused with a high efficiency. More importantly, because of the strong coordination between Pd and diamine ligands, Pd NPs could be anchored steadily over the support and only 5.0 ppm Pd residues was detected in products. This reaction was considered as pseudo-first order at high H 2 pressures, and the reaction activation energy was calculated to be as low as 18.1 kJ/mol. Our contribution is to provide an efficient and recyclable supported Pd catalyst, which may promote the development of heterogeneous catalytic systems for unsaturated macromolecular hydrogenation.
研究领域:
材料科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2024
·
IF 8.1
DePing Chen,ZhenYi Shao,LiRong Yang,Ying Chen,Yanghong Wei,Zhihua Hu,Liyang Cai,Yifan Zhang,Xun He
The design of efficient electrocatalysts for ethanol oxidation is essential for commercializing direct ethanol fuel cells (DEFCs). In this strategy, a mesoporous carbon microsphere (MC) was first synthesized by inverting the micro-emulsion technique. The MC@Au/Pd catalyst with a particular core-shell structure was obtained by utilizing mesoporous carbon as a core to load the Au/Pd layer. The novelty of the MC@Au/Pd catalyst with specialized core-shell structures lies not only in the high specific surface area inherited from the carbon core but also in the strong electronic interactions caused by the lattice mismatch between the core (Au) and shell (Pd) atoms. Particularly, electrochemical measures demonstrated that the Au/Pd catalyst exhibits superior catalytic activity toward the ethanol oxidation reaction (EOR) compared with commercial Pd/C catalysts. This is mainly due to the high specific surface area and mesoporous pore size inherited from the core carbon microspheres. In addition, the mesoporous carbon core and Au/Pd shell in the well-organized core-shell catalyst (MC@Au/Pd) influence the catalytic activity for ethanol oxidation by adjusting the electronic structure of Pd.
研究领域:
材料科学
·
能源化学
✓ 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）