JOURNAL OF CATALYSIS
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2019
·
IF 7.723
Jiaxuan Fan,Lingxiang Cheng,Yanan Liu,Yufei He,Yanfei Wang,Dianqing Li,Junting Feng
Photocatalytic reduction of CO 2 with H 2 O into CH 4 is a promising way to realize solar energy utilization and CO 2 conversion, in which the key issue is how to enhance and couple CO 2 reduction as well as H 2 O oxidation. In this work, we precisely fabricated a binary functional photocatalyst by loading Au@Pd nanoparticles onto V O -rich TiO 2 through a surfactant-free deposition-reduction method, whose fine structure was confirmed by aberration-corrected HAADF-STEM, EELS, EPR and XPS. Combining photocatalytic performance with a series of in situ FTIR measurements, we clarified the role of metallic sites and semiconductor support in coupling CO 2 reduction and H 2 O oxidation. Specifically, H 2 O oxidation process was facilitated by the V O -rich TiO 2 to contribute more protons, followed by the activation of CO 2 and protons primarily by the metallic Au@Pd sites to form the surface bounded Au@Pd-CO 2 − and Au@Pd-H species. By adjusting the ratio of Au@Pd nanoparticles and V O concentration to manipulate the Au@Pd-CO 2 − /Au@Pd-H ratio, CH 4 yield of 26.32 μmol/(g·h) and selectivity of electron toward CH 4 of 96% can be observed with minimal concomitant H 2 generation. These findings could open a feasible and universal route to enhance the photocatalytic efficiency of CO 2 conversion.
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ENERGY & FUELS
·
2019
·
IF 3.021
Lingjun Ma,Caixia Yue,Liang Ye,Qihuang Huo,Lina Han,Liping Chang,Weiren Bao,Jiancheng Wang
Pd–Fe bimetallic sorbents were shown to be a great potential sorbent for Hg0 removal from coal-derived fuel gas. In this work, activated carbon (AC), Al2O3, and Beta molecular sieve were chosen as supports to disperse Pd–Fe bimetallic components. The effects of the supports on Hg0 removal of Pd–Fe bimetallic sorbents were evaluated using a fixed-bed reactor at 200 °C. The regeneration performance of sorbents was also investigated. The results showed that Hg0 removal activity and regeneration performance over Pd–Fe/AC was the best, followed by Pd–Fe/Beta, and Pd–Fe/Al2O3. The Hg0 removal efficiency of Pd–Fe/AC bimetallic sorbents remained above 80% within 400 min after regeneration 4 times. The Pd–Fe bimetallic sorbents were characterized by N2 adsorption–desorption, Fourier transform infrared spectroscopy, X-ray diffraction, CO pulse adsorption, Hg temperature-programmed thermal desorption, and X-ray photoelectron spectroscopy. The analysis results revealed that three sorbents had a similar Hg0 removal mechanism. Hg0 transformed to Pd–Hg amalgam and HgS after reacting with the sorbents. Pd0 and Fe2O3 were the active species for the removal of Hg0. The removal performance of Hg0 by Pd–Fe/Al2O3 sorbents was the lowest. It is because Pd–Fe/Al2O3 sorbents have the lowest specific surface area, surface content, and dispersion degree of the Pd component. Furthermore, Pd0 over Pd–Fe/Al2O3 sorbents was severely poisoned and transformed to PdS during the regeneration process.
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Analytical Methods
·
2018
·Vol. 10
·期 11
·1331-1338
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IF 2.073
Huijuan Wang,Siyu Zhang,Shufang Li,Jianying Qu
Au@Pd core–shell nanoplates were synthesized successfully through the heterogeneous, epitaxial growth of Au on Pd nanoplates. The Pd nanoplates were prepared by reducing H2PdCl4 with PVP, and then served as seeds for the nucleation of Au atoms formed by reducing HAuCl4 with citric acid. Characterization of the as-prepared Au–Pd nanoplates by scanning electron microscopy revealed that a Au shell was formed around the Pd nanoplate. In order to avoid agglomeration, the Au@Pd nanoplates were loaded onto reduced graphene to give a Au@Pd/rGO nanohybrid, which exhibited excellent electrocatalytic activity towards the redox of hydroquinone (HQ) and catechol (CC) simultaneously. The linear detection ranges were 0.01–400.00 μM for HQ and 0.10–400.00 μM for CC, with detection limits of 0.01 μM for HQ and 0.10 μM for CC. Because of the excellent performance, lower detection, wider linear range, and better selectivity, the prepared Au@Pd/rGO nanohybrid has more potential applications and has an expected application in the electrochemical sensing field.
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JOURNAL OF MATERIALS SCIENCE
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2018
·Vol. 53
·期 21
·15064-15080
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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.
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ANALYTICA CHIMICA ACTA
·
2018
·
IF 5.123
Yamin Fu,Di Huang,Congming Li,Lina Zou,Baoxian Ye
This paper described a novel, facile and nonenzymatic electrochemical biosensor to detect hydrogen peroxide (H 2 O 2 ). The sensor was fabricated based on Pd-Pt nanocages and SnO 2 /graphene nanosheets modified electrode (PdPt [email protected] /GCE). The electrochemical behavior of PdPt [email protected] /GCE exhibited excellent catalytic activity toward H 2 O 2 with fast response, high selectivity , superior sensitivity, low detection limit of 0.3 μM and large linear range from 1 μM to 300 μM. Under these obvious advantages, the constructed biosensor provided to be reliable for determination of H 2 O 2 secreted from human cervical cancer cells (Hela cells). Hence, the proposed biosensor is a promising candidate for detection of H 2 O 2 in situ released from living cells in clinical diagnostics.
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JOURNAL OF CATALYSIS
·
2018
·
IF 6.759
Zhuo Zong,Kebin Xu,Dongliang Li,Zhenghua Tang,Wei He,Zhen Liu,Xiufang Wang,Yong Tian
Bimetallic core-shell nanostructures have been gaining considerable research attentions recently, mainly thanks to their versatile applications in many fields, including catalysis, electrocatalysis, electronic, sensing and so on. Herein, we demonstrate a peptide templated Au@Pd core-shell structure for both oxygen reduction reaction (ORR) and hydrogen evolution reaction (HER). By employing peptide sequence FlgA3 as surface capping agent, core-shell structure with Pd nanoparticles coated on the surface of Au nanoparticles were prepared. The Au@Pd core-shell structures demonstrated effective electrocatalytic activities toward both ORR and HER, whereas the catalytic activity was optimized by tuning the Pd-to-Au ratio. Among a series of samples tested, we discovered that the Au@Pd 1.0 sample exhibited the best ORR activity, superior to that of Pt/C and Pd/C, while its HER activity was also among the finest, close to that of Pt/C and Pd/C. The Au@Pd 1.0 sample also exhibited remarkable stability beyond Pt/C and Pd/C in both ORR and HER. Such intriguing electrocatalytic performances are attributed to the core-shell structure induced lattice strain. The results offer reliable pathway for designing peptide templated core-shell bimetallic nanostructures as dual or multiple functional electrocatalysts with excellent electrocatalytic activities and longevity.
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CATALYSIS LETTERS
·
2018
·Vol. 148
·期 7
·2019-2029
·
IF 2.911
Liu Anqiu,Huang Zhong,Wang Xiaochen
Abstract A new method has been developed for the oxidation of glucose into gluconic acid over Pd/C catalysts under the room temperature and atmospheric pressure. The carbon support was prepared by the hydrothermal treatment of renewable glucose, thus contained abundant active oxygen species. The Pd/C catalyst showed high catalytic activity towards the oxidation of glucose into gluconic acid. A 100% glucose conversion and a 98% gluconic acid yield were attained within 2 h at 0.1 MPa and room temperature. Structural analysis showed that the Pd paricle sizes of the catalysts were in the range of 10.1–16.2 nm influenced by the loading of Pd. The structure/size study showed that the catalyst with optimal particle size of 10.9 nm exhibited the highest TOF (0.2388 mol glucose mol Pd /s). The catalyst showed no significant loss of activity after recycled for four times. Graphical Abstract
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JOURNAL OF CATALYSIS
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2019
·
IF 7.723
Renshan Wang,Ganhua Qiu,Yi Xiao,Xueqin Tao,Wen Peng,Benxia Li
In this work, an all-solid-state Z-scheme photocatalyst of WO 3 ·H 2 O/Pd/CdS ternary heterostructures was constructed by introducing a small amount of Pd into the optimized WO 3 ·H 2 O/CdS binary system, where Pd nanoparticles (NPs) were sandwiched between WO 3 ·H 2 O nanosheets and CdS NPs. The WO 3 ·H 2 O/Pd/CdS ternary heterostructures exhibited remarkably enhanced photocatalysis towards the oxidative coupling of benzylamines to imines, compared with the other photocatalysts of WO 3 ·H 2 O, CdS, WO 3 ·H 2 O/CdS, WO 3 ·H 2 O/Pd, and WO 3 ·H 2 O/CdS/Pd. The wavelength-dependent photocatalysis of WO 3 ·H 2 O/Pd/CdS is in good agreement with its light-harvesting intensity at the corresponding wavelengths. The photoelectrochemical results reflected the enhanced charge carrier separation in WO 3 ·H 2 O/Pd/CdS, and the photocatalytic H 2 evolution confirmed the highly efficient Z-scheme charge transfer in this ternary photocatalyst. Therefore, the WO 3 ·H 2 O/Pd/CdS ternary heterostructures possess distinct advantages of extended light harvesting region, spatial separation of electron and holes, and elevated redox power, which synergistically contribute to the superior photocatalysis. The Pd NPs sandwiched between WO 3 ·H 2 O and CdS acted as not only an electron mediator to facilitate the interfacial charge separation but also a cocatalyst to accelerate the selective oxidation of benzylamine. This work demonstrates a rational design of highly efficient Z-scheme photocatalysts and presents some revelations about the photocatalytic mechanism for selective organic transformations.
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Catalysts
·
2018
·Vol. 8
·期 10
·443
·
IF 3.465
Kai Zheng,Chao Shen,Jun Qiao,Jianying Tong,Jianzhong Jin,Pengfei Zhang
Novel magnetically recyclable Fe3O4@Pd nanoparticles (NPs) were favorably synthesized by fixing palladium on the surface of nitrogen-doped magnetic nanocomposites. These catalysts were fully characterized by Fourier-transform infrared spectroscopy (FTIR), X-ray diffraction (XRD), transmission electron microscopy (TEM), thermogravimetric analysis (TG), and X-ray photoelectron spectroscopy (XPS). The prepared catalyst exhibited good catalytic activity for Suzuki–Miyaura coupling reactions of aryl or heteroaryl halides (I, Br, Cl) with arylboronic acids. These as-prepared catalysts could be readily isolated from the reaction liquid by an external magnet and reused at least ten times with excellent yields achieved. In addition, using this protocol, the marketed drug crizotinib (anti-tumor) could be easily synthesized.Keywords:heterogeneous catalyst;magnetically;palladium catalysts;nitrogen-doped;Suzuki coupling;crizotinib
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Nanomaterials
·
2019
·Vol. 9
·期 7
·1009
·
IF 4.034
Juanjuan Yin,Lun Zhang,Tifeng Jiao,Guodong Zou,Zhenhua Bai,Yan Chen,Qingrui Zhang,Meirong Xia,Qiuming Peng
With development of the society, the problem of environmental pollution is becoming more and more serious. There is the urgent need to develop a new type of sustainable green material for degradable pollutants. However, the conventional preparation method is limited by conditions such as cumbersome operation, high energy consumption, and high pollution. Here, a simple method named self-reduction has been proposed, to synthesize highly efficient catalytic nitro compounds and morin self-assembled MXene-Pd nanocomposites. Palladium nanoparticles were grown in situ on MXene nanosheets to form MXene@PdNPs. MXene@PdNPs composites with different reaction times were prepared by adjusting the reduction reaction time. In particular, MXene@PdNPs20 exhibited a high catalytic effect on 4-NP and 2-NA, and the first-order rate constants of the catalysis were 0.180 s−1and 0.089 s−1, respectively. It should be noted that after eight consecutive catalytic cycles, the conversion to catalyze 4-NP was still greater than 94%, and the conversion to catalyze 2-NA was still greater than 91.8%. Therefore, the research of self-assembled MXene@PdNPs nanocomposites has important potential value for environmental management and sustainable development of human health, and provides new clues for the future research of MXene-based new catalyst materials.Keywords:nanocomposites;catalyst;MXene;self-reduction;palladium nanoparticles
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高影响因子
ACS Applied Materials & Interfaces
·
2019
·
IF 8.456
Yicheng Zhong,Yuelin Mao,Shunli Shi,Mingming Wan,Chong Ma,Shuhua Wang,Chao Chen,Dan Zhao,Ning Zhang
MNPs@MOF catalysts obtained by encapsulating metal nanoparticles (NPs) into metal–organic frameworks (MOFs) show fascinating performance in heterogeneous catalysis. The improvement of catalytic activity and reusability of MNPs@MOF catalysts has been a great challenge for a long time. Herein, we demonstrate well-designed Pd/MOFs, featuring hollow double-shell structure and magnetic property, exhibiting high reusability, efficient catalytic activity, and size selectivity for hydrogenation reaction. The as-synthesized Pd/MOF, denoted as Void nFe3O4@Pd/ZIF-8@ZIF-8, possesses diverse functional structural features. The hollow cavity can improve mass transfer; superparamagnetic Fe3O4 NPs embedded in the inner MOF shell can enhance the separation and recyclability; Pd NPs are highly dispersed in the matrix of the inner MOF shell, and the outer MOF shell acts as a protector to prevent the leaching of Pd NPs and a sieve to achieve size selectivity. As a proof of concept, the Void nFe3O4@Pd/ZIF-8@ZIF-8 catalyst exhibited excellent performance for the hydrogenation of styrene at room temperature. The activity only reduced 10% after 20 cycles for the higher conversions (>90%), and the lower conversion only decreased 3.6% (from 32.5 to 28.9% conversion) after twenty consecutive cycles, indicating the good and intrinsic reusability of the catalyst. The proposed structure in this work provides a strategy to effectively improve the reusability of MNPs@MOF catalysts, which would increase their practical applications.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2025
·
IF 8.3
Jinxu Zhang,Fusheng Yang,Tao Fang,Bin Wang,Qingyuan Yang,Zhen Wu,Zaoxiao Zhang
The N-ethylcarbazole/dodecahydro-N-ethylcarbazole system, which offers advantages such as excellent hydrogen storage capacity, good reversibility, and reliable safety, is recognized as a potential candidate for hydrogen storage. However, the inefficient dehydrogenation by existing catalysts limits the commercial application of the system. In this work, CTAB was used as the soft template to increase the specific surface area of CeO 2 supports, and further the active metals were formed upon them through various reduction methods. A series of Pd/CeO 2 catalysts were thus prepared, among which Pd/CeO 2 –C6 adopted a composite strategy of using CTAB as the template to increase the specific surface area of CeO 2 and enhancing the dispersion of Pd through ultrasound assisted reduction, showed the best catalytic dehydrogenation performance for 12H-NEC. After 7 h of reaction at 453 K, the conversion rate of 12H-NEC reached 100 % with 97.24 % of hydrogen released. Combining BET, HRTEM, XPS, CO-pulse chemisorption and other characterization analyses, it was found that the incorporation of CTAB effectively enhanced both the specific surface area and oxygen vacancy concentration of CeO 2 , while ultrasound assisted reduction enabled a small particle size and good dispersion of metal Pd on the support. The strong synergetic effects of support and active metal in Pd/CeO 2 –C6 catalyst largely accounts for its good catalytic performance. This work offers valuable insights and guidance for the development of efficient dehydrogenation catalysts for 12H-NEC.
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