ChemCatChem
·
2014
·Vol. 6
·期 12
·3328-3332
·
IF 5.044
Xuan Xu,Haoran Li,Yong Wang
Graphical Being picky: N-Doped carbon (CN- x ) derived from N-containing ionic-liquid precursors are used as Pd nanoparticle supports for the selective hydrogenation of phenol to cyclohexanone with high activity and selectivity under mild reaction conditions. The activities of the Pd@CN- x catalysts derived from a variety of ionic liquids are different, and studies on the physical properties, Pd status, and N species of the catalysts are performed. In this report, a kind of mesoporous N-doped carbon (CN- x ) derived from N-containing ionic-liquid (IL) precursors were synthesized, and Pd@CN- x prepared by a simple ultrasound-assisted method showed higher catalytic activity for the selective hydrogenation of phenol and its derivatives under mild reaction conditions in water than commercial Pd@C and other common Pd heterogeneous catalysts. The catalytic activities of Pd@CN- x derived from different ILs were different, and further study into the influencing factors, including physical properties, N species of CN- x , and Pd status of Pd@CN- x , were performed.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2018
·
IF 4.229
Qing Qu,Guo-Liang Pan,Yan-Ting Lin,Chang-Wei Xu
High efficient and low-cost electrocatalysts for the oxygen evolution reaction (OER) are essential components of renewable energy technologies . However, the high onset potential and limited active sites restrict the catalytic activity of current electrocatalysts. Therefore, we are motivated by the development of cheap and efficient catalytic electrodes to promote the sluggish water-splitting systems associated with the large-scale application of clean and renewable energy technologies. Herein, a novel, simple, and efficient routine is presented by noble metal particles embedded within mesoporous metal oxide materials as high-efficiency anode catalysts for OER. Highly ordered mesoporous Co 3 O 4 was prepared by a nanocasting method using the silica KIT-6 as hard template, showing an enhanced electrochemical performance. Then, M - Co 3 O 4 (M = Pt, Pd, Au) nanomaterials were prepared by a simple but novel chemical reduction method. They show the high surface area of 112.3, 81.0 and 73.6 m 2 g −1 , which can provide more active surface area exposure leads to shorter paths of charges from electrolyte to electrode surface . Moreover, a three-dimensional highly ordered mesoporous structure can facilitate diffusion and penetration of electrolyte and oxygen, and can also keep catalyst nanoparticles in a well-dispersed condition with more active sites. Electrochemical measurements revealed that 20, 50, 25 wt% are the best weight contents for M (M = Pt, Pd, Au) in the Co 3 O 4 with highest electrochemical activity (0.410, 0.415 and 0.422 V vs. SCE) and j 0.7V reaching a maximum value. M-Co 3 O 4 (M = Pt, Pd, Au) materials exhibit superior activities and excellent long-duration stability in alkaline attributed to accelerating the formation of Co(IV) cations after being introduced M(M = Pt, Pd, Au) nanoparticles within mesoporous Co 3 O 4 . This kind of noble metal embedded within mesoporous oxide catalysts will hold a large potential as a highly promising electrocatalyst in the future.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2020
·
IF 16.683
Fukun Bi,Xiaodong Zhang,Jinfeng Chen,Yang Yang,Yuxin Wang
The highly dispersed Pd nanoparticles supported UiO-66 catalysts were successfully prepared via ethylene glycol reduction method (Pd-U-EG). And their catalytic performances were evaluated by toluene degradation. A series of characterization methods were carried out to characterize the physicochemical properties of the samples. During the effect of high weight hourly space velocity, stability and reusability test, the catalytic activity of Pd-U-EG remains unchanged, which also indicated good catalytic performance. More importantly, water resistance test (10-20 vol.% water) indicated that Pd-U-EG had a great water resistance. The study of toluene-TPD, toluene-TPSR and in-situ DRIFTS at different temperatures under different conditions over Pd-U-EG indicated the role of H 2 O. The introduction of H 2 O at low temperature was conducive to the adsorption of toluene, but inhibited the degradation of toluene. Differently, the H 2 O presence at high temperature was favorable to toluene degradation. In addition, toluene degradation mechanism was also revealed.
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ACS Sensors
·
2023
·
IF 8.9
Xuan-Yu Yang,Zheng-Guang Zhao,Li-Juan Yue,Ke-Feng Xie,Gui-Xin Jin,Shao-Ming Fang,Yong-Hui Zhang
Pd-based materials have received remarkable attention and exhibit excellent H2 sensing performance due to their superior hydrogen storage and catalysis behavior. However, the synergistic effects originated from the decoration of Pd on a metal oxide support to boost the sensing performance are ambiguous, and the deep investigation of metal support interaction (MSI) on the H2 sensing mechanism is still unclear. Here, the model material of Pd nanoparticle-decorated WO3 nanosheet is synthesized, and individual fine structures can be achieved by treating it at different temperatures. Notably, the Pd-WO3-300 materials display superior H2 sensing performance at a low working temperature (110 °C), with a superior sensing response (Ra/Rg = 40.63 to 10 ppm), high sensing selectivity, and anti-interference ability. DFT calculations and detailed structural investigations confirm that the moderate MSI facilitates the generation of high mobility surface O2– (ad) species and a proper ratio of surface Pd0–Pd2+ species, which can significantly boost the desorption of intermediate PdHx species at low temperatures and contribute to enhanced sensing performance. Our work illustrates the effect of MSI on sensing performance and provides insight into the design of advanced sensing materials.
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Scientific Reports
·
2017
·Vol. 7
·期 1
·1-10
·
IF 4.259
Wang Guojing,Jing Shengchang,Tan Yiwei
Shape control of noble metal (NM) nanocrystals (NCs) is of great importance for improving their electrocatalytic performance. In this report, branched Pd@Rh core@shell NCs that have right square prism-like arms with preferential exposure of Rh {100} facets (denoted as b-Pd@Rh-NCs thereafter) are synthesized and utilized as an electrocatalyst for the hydrazine electrooxidation (HEO) in acidic and alkaline electrolytes. The b-Pd@Rh-NCs are obtained by the heteroepitaxial growth of Rh on the pre-formed branched Pd NCs (denoted as b-Pd-NCs thereafter) core in the presence of poly(vinyl pyrrolidone) (PVP) and bromide ions. A comparative analysis of the voltammetric data for the HEO shows a higher activity on the b-Pd@Rh-NCs exposed with Rh {100} faces than on Rh black, the b-Pd-NCs, and Pd black in acid and alkaline solutions, indicating a structure sensitivity of the reaction. Analysis of the products from the b-Pd@Rh-NCs catalysed HEO reveals a very high hydrazine fuel efficiency, as determined by on-line differential electrochemical mass spectrometry (DEMS).
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ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Zaiyong Yang,Zhiheng Hao,Shunxin Zhou,Peng Xie,Zengxi Wei,Shuangliang Zhao,Fuzhong Gong
Direct synthesis of hydrogen peroxide (DSHP) from H2 and O2 offers a promising alternative to the present commercial anthraquinone method, but it still faces the challenges of low H2O2 productivity, low stability of catalysts, and high risk of explosion. Herein, by loading in a microchannel reactor, the as-synthesized Pd–Sn alloy materials exhibit high catalytic activity for H2O2 production, presenting a H2O2 productivity of 3124 g kgPd–1 h–1. The doped Sn atoms on the surface of Pd not only facilitate the release of H2O2 but also effectively slow down the deactivation of catalysts. Theoretical calculations demonstrate that the Pd–Sn alloy surface has the property of antihydrogen poisoning, showing higher activity and stability than pure Pd catalysts. The deactivation mechanism of the catalyst was elucidated, and the online reactivation method was developed. In addition, we show that the long-life Pd–Sn alloy catalyst can be achieved by supplying an intermittent flow of hydrogen gas. This work provides guidance on how to prepare high performance and stable Pd–Sn alloy catalysts for the continuous and direct synthesis of H2O2.
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Nanoscience and Nanotechnology Letters
·
2017
·Vol. 9
·期 6
·928-933
·
IF 1.889
Li Na,Feng Yahui,Du Jingjing,Li Changyun,Xie Shaowen,Xu Jianxiong
Hierarchically nanoporous Pd–HSiO1.5 particles were prepared by dissolving template method. The particles were analyzed by transmission electron microscope (TEM), nitrogen adsorption stripping curves, Barrett-Joyner-Halenda (BJH) pore size distribution curves and Fourier
Transform Infrared (FTIR). Hierarchically nanoporous Pd–HSiO1.5/Ni–Co composite electrodes were fabricated by the method of composite eletrodeposition using hierarchically nanoporous Pd–HSiO1.5 particles as composite nanoparticles. The electrocatalytic
activities for hydrogen evolution of the Ni–Co alloy electrodes and hierarchically nanoporous Pd–HSiO1.5/Ni–Co composite electrodes were studied. Results showed that the specific surface area and pore volume of nano-hierarchical porous silicon hydrogen compound
particles were 896 m2/g and 1.30 cm3/g respectively, the size of the hollow spheres was about 70 nm, and the thickness of the spherical shell was about 10 nm. In addition, the precious metal Pd was successfully loaded on the inside and surface of the hierarchically nanoporous
silicon hydrogen compound. The size of the inside Pd nanoparticles was about 3 nm, and the size of superficial Pd nanoparticles was 10–30 nm. The electrocatalytic hydrogen evolution performance of hierarchically nanoporous Pd–HSiO1.5/Ni–Co composite electrodes
was superior than that of Ni–Co alloy electrode, and the electrocatalytic activities of Pd–HSiO1.5/Ni–Co composite electrodes for hydrogen evolution reached the optimal value when the concentration of hierarchically nanoporous Pd–HSiO1.5 particles
was 1.8 g/L.
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JOURNAL OF CHEMICAL TECHNOLOGY AND BIOTECHNOLOGY
·
2019
·Vol. 95
·期 3
·862-874
·
IF 2.659
Fei Rao,Gangqiang Zhu,Miaomiao Wang,Siyaka Mj Zubairu,Jianhong Peng,Jianzhi Gao,Mirabbos Hojamberdiev
BACKGROUND Photocatalysis is one of the effective ways to solve the problem of water and gas pollution. An excellent photocatalyst should have the following advantages: efficient photocatalytic activity for gas and water pollutants, recyclable and stable characteristics, non-toxic and low-cost. Constructing heterojunctions and introducing oxygen vacancies (OVs) are two effective measures to achieve these targets. RESULTS It is found that the 1.0% Pd/PdO/β-Bi 2 O 3 exhibits the best photocatalytic activity with an efficiency of 97.4% for Bisphenol A (BPA) degradation and 47.6% for nitric oxide (NO) removal within 30 min. The 1.0% Pd/PdO/β-Bi 2 O 3 composite shows 23.3% efficiency in the photodegradation of BPA under 595 nm monochromatic light irradiation, while β-Bi 2 O 3 tends to be invalid. Moreover, the OVs promote the removal of NO without irradiation. CONCLUSION In this work, a novel ternary Pd/PdO/β-Bi 2 O 3 material as high-performance photocatalyst for the BPA degradation and NO removal was synthesized. The presence of OVs promotes the activation of the oxygen molecule, thereby facilitating the photocatalytic process. The p - n junction of PdO/β-Bi 2 O 3 and the Schottky barrier of Pd/β-Bi 2 O 3 significantly limit the recombination of photoinduced electron–hole pairs in the composite. Furthermore, an artifact in the electron spin resonance (ESR) spectrum obtained by spin trapping with 5,5-dimethyl-1-pyrroline N -oxide (DMPO) as adducts confirms that both hydroxyl radical (•OH) and superoxide radical (•O 2 − ) species are involved in the photocatalytic process. The present work offers a new perspective for developing the composite photocatalysts with high efficiency through loading of metal nanoparticles and creating an heterojunction. © 2019 Society of Chemical Industry
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2018
·
IF 3.141
Yuangong Zhang,Xin Wen,Yongqing Shi,Ru Yue,Libin Bai,Qingtao Liu,Xinwu Ba
Sulfur-containing polymer supported palladium nanoparticles (Pd/SPMB) were prepared by using the cross-linked poly(N,N′-methylene bis(acrylamide)) (SPMB) as the platform. The SPMB was synthesized via the reversible addition–fragmentation chain transfer (RAFT) polymerization, from which the sulfur inherently exists in the RAFT polymer due to the use of thiocarbonate as the chain transfer agent, and could be further utilized as a modifier of Pd nanoparticles. The Pd/SPMB showed size-dependent activity and selectivity in the semihydrogenation of alkynes to alkenes. The catalyst with an average Pd size of 5.3 nm was active in the semihydrogenation of both internal and terminal alkynes. Most of the surface of Pd NPs was covered (or poisoned) by sulfide and thiolate due to the moderate complexation strength between Pd NPs and SPMB, thus leading to the selectivity enhancement toward alkene. Furthermore, the catalyst was highly stable and can be reused 10 times without an appreciable loss in either activity or selectivity.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2021
·
IF 8.128
Qiong Wu,Lu Wang,Baozheng Zhao,Lang Huang,Shitao Yu,Arthur J. Ragauskas
A highly stable Pd-loaded N-doped carbon catalyst (ACN pd ) for phenol hydrogenation was prepared from chitosan by hydrothermal carbonization. ACN pd does not require a reduction step before catalytic use due to the Pd in the as-prepared catalyst mainly exists in the form of Pd 0 (80%). The carbon support involves N-containing groups such as pyridinic nitrogen and pyrrolic nitrogen, which could provide basic sites to adsorb phenol effectively. The as-fabricated ACN pd shows high catalytic performance with turnover frequency (TOF) of 29.34 h −1 . Accordingly, a phenol conversion of 100% and a cyclohexanone selectivity of 99.1% are achieved in 5 h at 100 °C and 1 MPa H 2 . This outstanding performance is attributed to the synergetic effects of the Pd particles, the N-functional groups, and the Lewis acid sites on the support. The carbon support presents intrinsic Lewis acid sites due to its electrophilicity, and Pd doping further increases the strength of such acid sites as it causes electron-deficient structural features. Moreover, the Lewis acid sites inhibit the over-hydrogenation from cyclohexanone to cyclohexanol. This study provides new insights into the application of functional biomass-based carbon materials as catalyst supports.
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CATALYSIS COMMUNICATIONS
·
2016
·
IF 3.389
Xingrui Fu,Yue Liu,Weiyuan Yao,Zhongbiao Wu
The catalytic performances of Pt-Pd/MCM-41 bimetallic catalysts prepared by one-step synthesis method were investigated for total toluene oxidation in this paper. The experimental results demonstrated that Pt-Pd/MCM-41 was of superior catalytic activity comparing to the monometallic Pt/MCM-41 or Pd/MCM-41 catalysts with the same metallic content, yielding an almost 100% conversion at 180 °C. The following characterization results indicated that the bimetallic catalyst possessed a higher surface Pt(0) content and smaller doped metal size owing to the synergistic effect of the two noble metals, resulting in the improvement of oxygen adsorption capacity and the reducibility.
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Catalysis Science & Technology
·
2022
·Vol. 12
·期 15
·4763-4775
·
IF 6.177
Ting Zhu,Ran Wang,Ziteng Chen,Feng Ji,Yuan Dong,Ming Yang
The problem of safe and efficient storage and transportation of hydrogen energy limits the large-scale development of the “hydrogen economy”. The liquid organic hydrogen storage technology is based on reversible catalytic hydrogenation and dehydrogenation reactions of unsaturated compounds to achieve safe and efficient storage and release of hydrogen. Heterogeneous catalysts with excellent catalytic capacity and stability should be developed to drive the reactions. However, it is a challenge to develop these catalysts. We fabricated a series of RuPd-based and supported catalysts following two different methods, and the catalytic hydrogenation and dehydrogenation activities of these catalysts were systematically investigated. The experiment results implied that the Pd2.5Ru2.5/H2 (double reduction method) catalyst exhibited catalytic hydrogenation rates that were similar to those of Pd2.5Ru2.5/L (when reduced by NaBH4). The former exhibited much better catalytic dehydrogenation rates than the latter. The Pd2.5Ru2.5/H2 catalyst also exhibited much better catalytic recyclability than the Pd2.5Ru2.5/L catalyst, and the conclusion was arrived at by conducting 10 cycles of hydrogenation–dehydrogenation tests. The relationship between the catalytic performances and the catalyst's properties was further investigated using a combination of H2-TPR, NH3-TPD, XPS, and TEM techniques. The characterization results revealed that the double reduction process could be used to enhance the extent of electronic interaction of the RuPd active sites with the support, and more numbers of strong acidic sites and active sites could be generated. Furthermore, DFT calculations also revealed that 8H-NPCZ and 4H-NPCZ formed stable adsorption structures on the Ru3Pd3/Al2O3(100) surface, facilitating catalytic reactions. Notably, the reaction energies of Ru3Pd3/Al2O3(100) were 1.16 eV, 1.42 eV, and 1.63 eV, indicating that the dehydrogenation process (8H-NPCZ → 4H-NPCZ and 4H-NPCZ → NPCZ) occurred easily. All the above-mentioned characteristics make the Pd2.5Ru2.5/H2 catalyst an excellent catalyst for hydrogenation and dehydrogenation and endow it with outstanding catalytic capacity and recyclability.
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