APPLIED SURFACE SCIENCE
·
2025
·
IF 6.9
Ruichun Nan,Xinxin Zhang,Yuheng Zhao,Hongda Huang,Yapeng Niu,Ying Yan,Litao Zhang,Bingkun Liu,Jingtao Zhang,Xianzhong Yin
Herein, Pd-doped CeO 2 was synthesized by facile hydrothermal methods, X-ray diffraction (XRD) analysis and transmission electron microscope (TEM) suggests that Pd is successfully incorporated into the CeO 2 lattice. X-ray photoelectron spectroscopy (XPS), UV–Vis and PL demonstrated that Pd-doped CeO 2 improve the light absorption and enhance the electron-hole separation of CeO 2 . The prepared Pd-CeO 2 exhibits outstanding bactericidal performance. Specifically, 1 % Pd-CeO 2 can completely inactivate Ralstonia solanacearum with an initial concentration of 2 × 10 7 CFU/mL within 60 min, while also demonstrating effective killing against Escherichia coli and various pathogenic fungi. EPR demonstrated that Pd doping into CeO 2 could increase the number of vacancies, electron spin resonance (ESR) tests demonstrated that e - play a major role in the photocatalytic process, disruption of the cellular structure of E. coli during photocatalytic treatment as evidenced by scanning electron microscopy (SEM) tests. Promising reference for the practical application of precious metal photo catalysts in disinfection.
研究领域:
材料科学
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微生物学
·
环境科学
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产品关联
DOI
高影响因子
ELECTROCHIMICA ACTA
·
2020
·
IF 6.215
Hui Jiang,Lin Liu,Kai Zhao,Zhen Liu,Xinsheng Zhang,Shuozhen Hu
Nitrogen doping was widely used to increase the electronic density of carbon materials and to enhance the adsorption of the supported metal catalysts . However, the exact interaction between various doped nitrogen species and palladium (Pd) have rarely been reported for formic acid electrooxidation (FAO). In this study, the effect of the doped pyridinic-N and pyrrolic-N on the electronic structure and the electrochemical activity of Pd toward FAO are investigated. The oxidation state of Pd is reduced and more metallic Pd is formed when Pd nanoparticles supported on pyridinic-N and pyrrolic-N doped carbon materials . Density functional theory (DFT) calculations simulate that the adsorption energy of HCOO* and *COOH on Pd/pyrrolic-N are lower than those on Pd/pyridinic-N. Both DFT and electrochemical measurements suggest that the FAO activity of Pd is more correlated with the pyrrolic-N than pyridinic-N. The catalyst contains more pyrrolic-N species exhibits higher electrochemical activity and faster kinetics for FAO reaction. Moreover, Pd 2+ -N complexes are formed in all the nitrogen doped catalysts and display good activity for FAO. In this study, Pd supported on urea treated carbon (Pd/UR) owns the highest content of pyrrolic-N and exhibits the best activity for FAO.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
JOURNAL OF CATALYSIS
·
2018
·
IF 6.759
Yujie Song,Hao Wang,Shijing Liang,Yan Yu,Liuyi Li,Ling Wu
The photoalkylation of nitroarenes with benzyl alcohols in one pot at room temperature and 1 atm N 2 was achieved over the Pd/H 1.07 Ti 1.73 O 4 ·H 2 O nanosheets. The sample shows efficient photocatalytic activity with high conversion of nitrobenzene (99%) and selectivity of secondary amine (85%). This flexible photocatalytic system is also applicable to other nitroarenes with high efficiency. Results of in situ FTIR, DRS, and in situ ESR revealed that the benzyl alcohol and nitrobenzene molecules can bind with the surface Lewis and Brønsted acid sites in the catalyst via the H O⋯Ti and NO 2 ⋯H O Ti species. The formation of surface coordination species results in not only the activation of reactant molecules via surface electron transfer, but also the expanded visible light absorption of the catalyst. Moreover, in situ ESR suggested that the surface coordination can also facilitate the formation of oxygen vacancies in catalysts, which can greatly promote the exposure of Lewis sites and enhance the activation of reactant molecules. Finally, a possible hydrogen transfer strategy over the sample is proposed on a molecular level.
研究领域:
化学
·
材料科学
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产品关联
DOI
高影响因子
JOURNAL OF MOLECULAR STRUCTURE
·
2020
·
IF 2.463
Shaoping Feng,Kun Huang,Zhangjie Huang,Guiyang Liu,Guowei Zhang,Gaozhang Gou
ABSTRACT In view of the separation and recycling of Pd(II) from multi-metal aqueous solution, a functionalized extractant of 2-[(2-ethylhexyl)thio]benzoxazole (EHBXS) with excellent selectivity for Pd(II) was synthesized and used to extract Pd(II) for the first time. The effects of EHBXS concentration, HCl concentration, organic/aqueous (O/A) phase ratio, contact time, and regeneration of EHBXS were investigated in detail. The extraction efficiency of Pd(II) was almost 100 % while the co-extraction efficiencies of Pt(IV), Rh(III), Cu(II), Fe(III) and Ni(II) existed in the aqueous solution were less than 10 %, which indicates that EHBXS is an effective extractant and can effectively remove Pd(II) from other metals at desired extraction conditions. Thiourea ((NH 2 ) 2 CS) solution (1.0 mol/L) could be used as an effective Pd(II) stripping agent and the one-step stripping efficiency of Pd(II) was higher than 98 %. EHBXS has excellent regeneration ability and the extraction efficiency of Pd(II) with regenerated EHBXS reaches to 87% even after 7 cycles. Moreover, the coordination mechanism between EHBXS and Pd(II) has been proven via the slope method, FT-IR spectra, 1 H NMR, 13 C NMR and single X-ray diffraction. Pd(II) and EHBXS formed a 1:2 complex of Pd(EHBXS) 2 Cl 2 during extraction. Pd(II) was coordinated with two Cl atoms and two EHBXS, and thus formed Pd(EHBXS) 2 Cl 2 molecule, in which EHBXS was coordinated with Pd(II) via the N atom in the benzoxazole ring as neutral unidentate ligand.
研究领域:
化学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION SCIENCE AND TECHNOLOGY
·
2018
·
IF 1.2
Yan Yan,Qi Wang,Zeyang Xiang,Yanzhao Yang
A reasonable project was presented for the extraction and separation of Pt(IV), Pd(II), Ru(III), and Rh(III) from the mixed imidazolium-based ionic liquids (ILs) [C6mim]Cl, [C6mim][NTf2], and [C6mim][DDTC]. Pt(IV) was first separated from other three platinum group metals with a mixture of [C6mim]Cl and [C6mim][NTf2]. Then, separation of Pd(II) and Ru(III) from Rh(III) was realized by changing the concentration of [C6mim][DDTC]. Back-extraction of Pt(IV), Pd(II), and Ru(III) from loaded hydrophobic phase and the recovery of Rh(III) in aqueous phase were also investigated. Mechanisms between Pd(II)/Ru(III) and [C6mim][DDTC] were further explored using ultraviolet spectrophotometry (UV-Vis), infrared spectrophotometry (FTIR), the method of continuous variations, ab initio quantum chemical studies, and X-ray crystallographic analysis. The results afford more directions for extracting and separating metals by introducing devisable functionalized group into ILs.
研究领域:
化学工程
·
分析化学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Nanxing Gao,Dongchen Han,Tongtong Yang,Qinglei Meng,Xian Wang,Changpeng Liu,Junjie Ge,Wei Xing
The importance of the dynamic structural evolution of water in the solid–liquid interface cannot be overstated. However, the ubiquitous hydrogen-bonded network is notoriously difficult to probe owing to complex interfacial environment. Formic acid , a fair hydrogen-bond donor and acceptor, is a promising reversible hydrogen storage/release material. Herein, isotope-labeled in-situ mass spectrometry (MS) and operando surface-enhanced Fourier transform infrared measurements ( operando FT-IR) reveal the central role of water during formic acid dehydrogenation . The water-promoted restructured HCOONa-Pd@ANI/C catalyst exhibits 100% selectivity, 100% conversion yield with high stability (even after 112 days) under ambient conditions. Coupled to a proton exchange membrane fuel cell, this integrated system reaches a high power density at 29.81 W⋅g Pd −1 . Our study demonstrates a new pathway involving water, the indispensable proton transfer and exchange through efficiently hydrogen-bonded network in light of operando experimental evidence.
研究领域:
催化化学
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材料科学
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表面化学
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产品关联
DOI
高影响因子
DALTON TRANSACTIONS
·
2017
·Vol. 46
·期 22
·7210-7218
·
IF 4.029
Wenhui Liu,Qi Wang,Yan Zheng,Shubin Wang,Yan Yan,Yanzhao Yang
In this study, a method of one-step separation and recycling of high purity Pd(II) and Pt(IV) using an ionic liquid, 1-butyl-3-benzimidazolium bromate ([HBBIm]Br), was investigated. The effects of [HBBIm]Br concentration, initial metal concentration, and loading capacity of [HBBIm]Br were examined in detail. It was observed that [HBBIm]Br was a very effective extractant for selectively extracting Pd(II) and precipitating Pt(IV). Through selectively extracting Pd(II) and precipitating Pt(IV), each metal with high purity was separately obtained from mixed Pd(II) and Pt(IV) multi-metal solution. The method of one-step separation of Pd(II) and Pt(IV) is simple and convenient. The anion exchange mechanism between [HBBIm]Br and Pt(IV) was proven through Job's method and FTIR and 1H NMR spectroscopies. The coordination mechanism between [HBBIm]Br and Pd(II) was demonstrated via single X-ray diffraction and was found to be robust and distinct, as supported by the ab initio quantum-chemical studies. The crystals of the [PdBr2 ·2BBIm] complex were formed first. Moreover, the influence of the concentrations of hydrochloric acid, sodium chloride, and sodium nitrate on the precipitation of Pt(IV) and extraction of Pd(II) was studied herein. It was found that only the concentration of H+ could inhibit the separation of Pt(IV) because H+ could attract the anion PtCl62−; thus, the exchange (anion exchange mechanism) between the anions PtCl62− and Br− was prevented. However, both the concentration of H+ and Cl− can obviously inhibit the extraction of Pd(II) because H+ and Cl− are the reaction products and increasing their concentration can inhibit the progress of the reaction (coordination mechanism).
研究领域:
化学
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材料科学
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产品关联
DOI
PubMed
高影响因子
APPLIED ORGANOMETALLIC CHEMISTRY
·
2017
·Vol. 31
·期 12
·e3889
·
IF 2.319
Tao Feng,Ranxiao Tang,Ningzhao Shang,Cheng Feng,Shutao Gao,Chun Wang
A facile and efficient method for facilitating hydrogen generation from formaldehyde aqueous solution was developed using Pd nanoparticles supported on CeO 2 (Pd/CeO 2 ) as the catalyst. The prepared Pd/CeO 2 catalyst exhibited 100% H 2 selectivity and excellent catalytic activity for formaldehyde dehydrogenation with the initial rate of 2089 ml min −1 g Pd −1 at room temperature and atmospheric pressure without any extra additive. The prepared catalyst was stable and reusable, and its catalytic activity kept almost unchanged after it was reused for the fifth run. Therefore, it is considered that this Pd/CeO 2 based hydrogen generation system may serve as an alternative hydrogen supply candidate for practical application.
研究领域:
化学
·
能源材料科学
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产品关联
DOI
高影响因子
CATALYSIS LETTERS
·
2015
·Vol. 146
·期 1
·117-125
·
IF 2.307
Dong Wenhuan,Feng Cheng,Zhang Li,Shang Ningzhao,Gao Shutao,Wang Chun,Wang Zhi
Abstract
In this paper, the palladium nanoparticles were successfully encapsulated in metal–organic framework material, UiO-66, by a facile approach. Based on the microwave-assisted method, the pores of UiO-66 were activated and the metal precursors were reduced at the same time in the presence of reducing agent. The obtained Pd@UiO-66 was characterized via transmission electron microscopy, powder X-ray diffraction, N 2 adsorption and X-ray photoelectron spectroscopy. The Pd@UiO-66 exhibited efficient catalytic activity for the Suzuki–Miyaura coupling reactions at mild condition. Graphical Abstract The palladium nanoparticles were successfully encapsulated in metal–organic framework material, UiO-66, by a facile approach. Based on the microwave-assisted method, the pores of UiO-66 were activated and the metal precursors were reduced at the same time in the presence of reducing agent. The obtained Pd@UiO-66 exhibited efficient catalytic activity for the Suzuki–Miyaura coupling reactions at mild condition.
研究领域:
材料科学
·
化学
✓ 已验证
产品关联
DOI
高影响因子
Energy & Environmental Materials
·
2021
·Vol. 6
·期 1
·e12292
·
IF 15.122
Ruofan Shen,Yanyan Liu,Hao Wen,Xianli Wu,Zhikun Peng,Sehrish Mehdi,Tao Liu,Huanhuan Zhang,Shuyan Guan,Erjun Liang,Baojun Li
The dissociation of water is the rate-determining step of several energy-relating reactions due to high energy barrier in homolysis of H-O bond. Herein, engineering vacancy-atom ensembles via injecting oxygen vacancy (V O ) into single facet-exposed TiO 2 -Pd catalyst to form V O -Pd ensemble is proposed and implemented. The outstanding activity of as-prepared catalyst, 1.5-PdTV O , toward water dissociation is established with a turnover frequency of 240 min −1 in ammonia borane hydrolysis at 298 K. Density functional theory simulation suggests that the V O -Pd ensemble is responsible for the high intrinsic catalytic activity. Water molecules tend to be dissociated on V O sites and ammonia borane molecules on Pd atoms. Those H atoms from water dissociation on V O combine with H atoms from ammonia borane on Pd atoms to generate H 2 . This insights into engineering vacancy-atom ensembles catalysis provide a new avenue to design catalytic materials for important energy chemical reactions.
研究领域:
材料科学
·
催化化学
·
能源化学
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产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2023
·
IF 7.2
Huanhuan Zhang,Qunying Sun,Linyan Bian,Qiuming Peng,Shumin Han,Baozhong Liu,Yanping Fan
Developing noble-based catalysts with high activity is the key to realizing high-efficiency hydrogen generation. Herein, PdRh alloys with different ratios supported on active Ti 3 C 2 is designed by microwave-assisted reduction to enhance the dissociation of NH 3 BH 3 and H 2 O. Specially, Pd 1 Rh 4 /Ti 3 C 2 conveys an optimal turnover frequency ( TOF ) of 338 min −1 and activation energy ( E a ) of 33.8 kJ mol −1 at room temperature. The TOF of Pd 1 Rh 4 /Ti 3 C 2 is 7.3 times than that of Pd/Ti 3 C 2 and 4.8 times of Rh/Ti 3 C 2 because of the construction of dual-active sites of PdRh alloy and active Ti 3 C 2 . The introduction of a small number of Pd changes the chemical environment of catalysts and presents significant excitation effect on catalytic activity. Experimental investigation reveals PdRh alloy and active Ti 3 C 2 are beneficial for the adsorption and dissociation of NH 3 BH 3 and H 2 O (active Ti 3 C 2 activates H 2 O, PdRh activates NH 3 BH 3 ). This research provides experimental foundation for the design of noble-based catalysts with high catalytic activity.
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
JOURNAL OF CATALYSIS
·
2024
·
IF 6.5
Hang Li,Kaisheng Yao,Tianhang Liu,Tianhang Han,Qi Wang,Aozhou Wang,Weiwei Lu
Bimetallic AuPd plasmonic photocatalyst is a promising candidate for catalyzing selective oxidation of aromatic alcohol. However, developing a simple one-step method for the preparation of free-standing AuPd nanostructures with excellent photocatalytic performance remains a huge challenge. Here, a facile liquid–liquid interface route was exploited to one-pot prepare free-standing AuPd alloy nanowires (NWs) under mild conditions. Specifically, Au 1 Pd 1 NWs are grown via oriented attachment at chloroform-water interface and 40 °C with Na 2 PdCl 4 and HAuCl 4 as precursors and 1-naphthol as reductant. Au 1 Pd 1 NWs possess many advantages, such as thin diameter (4.0 nm), large aspect ratio, abundant defects and strong Au-Pd electronic interaction. During benzyl alcohol oxidation to benzaldehyde, Au 1 Pd 1 NWs exhibit excellent photocatalytic activity and durability. At 40 min of visible light illumination, 98 % conversion of benzyl alcohol and 100 % selectivity to benzaldehyde are finished. After five cycles, Au 1 Pd 1 NWs still maintain high photocatalytic activity. Compared to pure Au NWs, alloying Pd with Au in Au 1 Pd 1 NWs dramatically enhances photocatalytic activity. The results indicate that the generated abundant •O 2 – under illumination play an important role in significantly improving benzyl alcohol oxidation to benzaldehyde.
研究领域:
材料科学
·
催化化学
·
纳米技术
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）