Catalysts
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2018
·Vol. 8
·期 5
·200
·
IF 3.465
Shiying Han,Yunfei Liu,Jiang Li,Rui Li,Fulong Yuan,Yujun Zhu
A series of Pd-Ni bimetallic catalysts supported on SBA-15 (0.2%Pd-x%Ni/SBA-15, x = 0.4, 0.7, and 1.2) were prepared through the impregnation method combined with the NaBH4reduction method. X-ray diffraction (XRD), N2adsorption-desorption, X-ray photoemission spectroscopy (XPS) and transmission electron microscope (TEM) were used to characterize the prepared catalysts. All the synthesized catalysts were evaluated for the liquid-phase hydrogenation of cinnamaldehyde (CAL). The addition of Ni obviously enhanced the CAL conversion and selectivity of C=C hydrogenation to hydrocinnamaldehyde (HALD) over the 0.2%Pd-x%Ni/SBA-15 catalysts. Meanwhile, 0.2%Pd-1.2%Ni/SBA-15 showed the best performance with 96.3% conversion and 87.8% selectivity toward HALD. This improvement was attributed to the synergistic effect between the Pd and Ni nanoparticles, enhancing the dispersion of Pd metal particles and increasing the content of surface Pd0species. In addition, the influences of a few reaction factors including H2pressure, reaction temperature, and reaction time were studied over 0.2%Pd-1.2%Ni/SBA-15.Keywords:selective hydrogenation;cinnamaldehyde;hydrocinnamaldehyde;synergistic effect;Pd-Ni/SBA-15
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JOURNAL OF CATALYSIS
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2018
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IF 6.759
Bing Hu,Yazhi Yin,Guoliang Liu,Shengli Chen,Xinlin Hong,Shik Chi Edman Tsang
Surface modification with Pd is an effective way for improved activity in CO 2 hydrogenation to methanol over commercial Cu-ZnO catalysts via a so-called hydrogen spillover mechanism. However, there still lacks a quantitative analysis of hydrogen spillover effect and the nature of active sites after Pd modification remains unclear. In this work, we prepared a series of Pd-doped Cu-ZnO catalysts (Pd-CZ-x) with tunable Pd loading by using a facile polyol reduction method for a deep study of the promotion effect of Pd. With the increase of Pd/Cu molar ratio (x) from 0 to 0.04, there emerges a volcano-shaped relationship between methanol space time yield (STY) and Pd loading. 1% Pd doping can increase the methanol STY by 2.5 times and the methanol turnover frequency (TOF) by 3.5 times at 543 K, when compared to undoped Cu-ZnO. Kinetic studies show the activation energy required for methanol synthesis is greatly reduced from 59 kJ mol −1 over Cu-ZnO to 31 kJ mol −1 over Pd-CZ-0.01. Behind the volcano-shaped relationship is a balance between the hydrogen spillover effect of Pd and the reduced surface Cu area caused by Pd blocking. Chemisorption gives a quantitative analysis of an important type of activated Cu sites enabled by hydrogen spillover (Cu hs ). Importantly, it is found that the methanol STY correlates linearly with Cu hs surface area, suggesting that the activated Cu sites with the assistance of ZnO are real active sites for methanol synthesis from CO 2 hydrogenation.
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Catalysis Science & Technology
·
2018
·Vol. 8
·期 13
·3238-3245
·
IF 5.365
Hongxu Yan,Yunyi Liu,Tao Zhang,Ze Jin,Ming Wang,Ying Peng Xie,Hongfan Guo
Pd catalysts, which are often prepared by reducing Pd salts with NaBH4, have been intensely studied in HCOOH dehydrogenation (FAD) for H2 production. FAD can also be used to hydrogenate or reduce various chemicals by using its in situ generated hydrogen, which exhibits superiority over the direct use of H2 gas. Herein, by using FAD to reduce Cr(VI) as a room-temperature probe reaction, we show that some Pd atoms in the catalyst form PdHx under normal conditions during both catalyst preparation and catalytic reaction (NaBH4 or HCOOH as a hydrogen donor). PdHx greatly hinders Cr(VI) reduction and, interestingly, boosts H2 generation. That is to say, PdHx can be negative or positive species, depending on the focused product. The reason for this phenomenon was also analyzed. Heat treatment for only 10 min can destroy PdHx species and thus, improve the activity for Cr(VI) reduction by up to ∼3 times, which is effective in each catalyst reuse. These findings are critical for controlling the design and functioning of Pd catalyst.
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ECOTOXICOLOGY AND ENVIRONMENTAL SAFETY
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2018
·
IF 3.974
Zhuyu Niu,Yating Jia,Yuancai Chen,Yongyou Hu,Junfeng Chen,Yuancai Lv
This study constructed a biological-inorganic hybrid system including Pseudomonas putida ( P. putida ) and bioreduced Pd (0) nanoparticles (NPs), and inspected the influence of bio-nano Pd (0) on the direct electron transfer and phenol biodegradation. Scanning electron microscopy and energy-dispersive X-ray spectroscopy (SEM-EDX) showed that bio-nano Pd (0) (~10 nm) were evenly dispersed on the surface and in the periplasm of P. putida . With the incorporation of bio-nano Pd (0), the redox currents of bacteria in the cyclic voltammetry (CV) became higher and the oxidation current increased as the addition of lactate, while the highest increase rates of two electron transfer system (ETS) rates were 63.97% and 33.79%, respectively. These results indicated that bio-nano Pd (0) could directly promote the electron transfer of P. putida . In phenol biodegradation process, P. putida -Pd (0)− 2 showed the highest k (0.2992 h −1 ), μ m (0.035 h −1 ) and K i (714.29 mg/L) and the lowest apparent K s (76.39 mg/L). The results of kinetic analysis indicated that bio-nano Pd (0) markedly enhanced the biocatalytic efficiency, substrate affinity and the growth of cells compared to native P. putida . The positive effects of bio-nano Pd (0) to the electron transfer of P. putida would promote the biodegradation of phenol.
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CHEMICAL ENGINEERING JOURNAL
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2017
·
IF 6.216
Gang Chen,Xun Zhu,Rong Chen,Qiang Liao,Dingding Ye,Hao Feng,Jian Liu,Ming Liu
Unlike traditional gas–liquid–solid microreactors with the catalyst coated on the inner wall, a gas–liquid–solid monolithic microreactor with the Pd nanocatalyst coated on the polydopamine modified nickel foam was developed in this study. This new design enables large surface area for loading the nanocatalyst and enhancement of mass transfer. The performance of the proposed monolithic microreactor was evaluated by hydrogenation of nitrobenzene. It was found that this monolithic microreactor displayed more excellent performance than conventional flat microreactor. Meanwhile, the effects of the nickel foam length, liquid flow rate, gas flow rate and inlet nitrobenzene concentration on the nitrobenzene conversion, aniline concentration at the outlet and gas conversion were also studied. Experimental results showed that the increase of the nickel foam length and gas flow rate and the decrease of the liquid flow rate could improve the performance. Besides, although increasing the inlet nitrobenzene concentration could result in the increased aniline concentration at the outlet and gas conversion but the nitrobenzene conversion was decreased. This work opens a new window for the design of high-performance gas–liquid–solid microreactor toward multiphase catalytic reactions.
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JOURNAL OF SOLID STATE ELECTROCHEMISTRY
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2017
·Vol. 22
·期 3
·817-824
·
IF 2.316
Liu Yong,Li Shenshen,Zhang Yunmao,Liu Weihua,Wang Jianhong,Zhai Cuiping
Honeycomb-like porous carbons (PCs) were synthesized using a facile self-assembly method with phenolic resin as the carbon source and tetraethyl orthosilicate (TEOS) as the silica source. The PCs were found to have a large BET surface area of 458 m 2 g −1 and a partially graphitized structure. The obtained PCs were used as a support for various Pt-Pd bimetallic alloy catalysts employed for methanol oxidation in alkaline media. Compared with Pt supported on commercial Vulcan XC-72R carbon (Pt/C) and with the other Pt-Pd bimetallic alloy catalysts on PCs, Pt 3 Pd 1 on PCs displayed the most negative onset potential for methanol oxidation and the highest steady-state current (2.04 mA cm −2 ). This may be because the Pt 3 Pd 1 /PCs catalyst has the largest electrochemical active surface area (ESA), and because adding Pd to the catalyst improves the ability of the intermediate species to tolerate oxidation. The results show that the prepared Pt-Pd/PCs is a potential candidate for application as a catalyst in alkaline direct methanol fuel cells.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
·
IF 9.4
Zhiang Hou,Hao Chen,Jiangfeng Chu,Jinnan Wang,Aimin Li,Philippe François-Xavier Corvini
Herein, the bimetallic Pd 3 In 1 alloy were deposited onto the crystal facet engineered TiO 2 nanosheet (NS) via one-step photoreduction (Pd 3 In 1 /TiO 2 -NS) for selective conversion of nitrate (NO 3 − ) to N 2 . Bimetallic Pd 3 In 1 provides higher affinity sites to bind NO 3 − and significantly reduces the energy barrier of the rate-limiting step (NO 3 * + e − → NO 2 *), which is the key for the ultra-fast NO 3 − reduction kinetics. More importantly, the synergistic effect of Pd and In not only suppresses the hydrogen evolution reaction resulting in high efficiency utilization of photogenerated electrons, but also promotes the selective conversion of nitrite (NO 2 − ) to N 2 . Consequently, Pd 3 In 1 /TiO 2 -NS exhibits 100 % NO 3 − conversion and 90 % N 2 selectivity within 20 min in six cycles. One order of magnitude improvement on the NO 3 − reduction kinetic constants of Pd 3 In 1 /TiO 2 -NS (0.254 min −1 ) is achieved compared with pristine TiO 2 -NS and monometallic loaded ones. This work provides new insights into the rational construction of bimetallic alloy cocatalysts for high-efficiency photocatalytic denitrification.
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ACS Nano
·
2024
·
IF 15.8
Shizhen Geng,Pengke Guo,Xinling Li,Yaru Shi,Jing Wang,Mengnian Cao,Yunya Zhang,Kaixiang Zhang,Airong Li,Haiwei Song,Zhenzhong Zhang,Jinjin Shi,Junjie Liu,Yiling Yang
Immune checkpoint blockade (ICB) therapy has been approved for breast cancer (BC), but clinical response rates are limited. Recent studies have shown that commensal microbes colonize a variety of tumors and are closely related to the host immune system response. Here, we demonstrated that Fusobacterium nucleatum (F.n), which is prevalent in BC, creates an immunosuppressive tumor microenvironment (ITME) characterized by a high-influx of myeloid cells that hinders ICB therapy. Administering the antibiotic metronidazole in BC can deplete F.n and remodel the ITME. To prevent an imbalance in the systemic microbiota caused by antibiotic administration, we designed a biomimetic nanovehicle for on-site antibiotic delivery inspired by F.n homing to BC. Additionally, ferritin-nanocaged doxorubicin was coloaded into this nanovehicle, as immunogenic chemotherapy has shown potential for synergy with ICB. It has been demonstrated that this biomimetic nanovehicle can be precisely homed to BC and efficiently eliminate intratumoral F.n without disrupting the diversity and abundance of systemic microbiota. This ultimately remodels the ITME, improving the therapeutic efficacy of the PD-L1 blocker with a tumor inhibition rate of over 90% and significantly extending the median survival of 4T1 tumor-bearing mice.
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JOURNAL OF MATERIALS CHEMISTRY
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2012
·Vol. 22
·期 18
·9117-9122
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IF 5.968
Sha Chen,Hongye Zhang,Lingyan Wu,Yanfei Zhao,Changliang Huang,Maofa Ge,Zhimin Liu
Based on the galvanic replacement reaction between Cu nanoparticles and noble metal ions, a simple and efficient strategy was developed for the preparation of supported Cu–M (M = Pt, Pd, Ru, Rh) bimetallic nanoparticles under intense ultrasonication irradiation at ambient environment. A series of Cu–M/TiO2 bimetal catalysts with controllable composition, metal particle size less than 2 nm and narrow size distribution were obtained, and characterized by transmission electron microscopy (TEM), high resolution transmission electron microscope (HRTEM) with scanning TEM (STEM) mode, energy-dispersive X-ray spectrometers (EDS), X-ray photoelectron spectroscopy (XPS), X-ray diffraction (XRD), and ICP-AES analysis. It was demonstrated that most of the metal particles were present in the form of bimetallic state. The mechanism of this strategy was discussed. The resultant Cu–Pd/TiO2 was used to reduce nitrate at room temperature, and it exhibited extremely high activity.
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Journal of Energy Storage
·
2024
·
IF 8.9
Congwen Duan,Haimei Wang,Jinhui Wu,Ting Qu,Yuling Zhang,Dong Fu,Lianxi Hu,Fei Wang,Dongsheng Lai,Yueru Dai,Ying Wu
Mg/MgH 2 stands out as an excellent hydrogen storage material due to its abundant presence and its capacity for high hydrogen storage density. However, the sluggish hydrogenation/dehydrogenation kinetics make it unsuitable for solid-state hydrogen storage. To tackle these challenges, the MgH 2 -Co@Pd‑c arbon nanotubes composite was created through ball milling , and its hydrogenation/dehydrogenation behavior was examined. The inclusion of Co@Pd notably enhanced the kinetics of hydrogenation/dehydrogenation in Mg/MgH 2 . The Mg-Co@Pd‑c arbon nanotubes composite achieved an absorption of 7.30 wt% H 2 in just 8 h of milling. The study proposed an energy conversion model to investigate the enhanced properties of Mg/MgH 2 . The addition of Co@Pd substantially reduced the activation energy (Ea) for hydrogen desorption to 81.9 kJ/mol. Furthermore, Transmission Electron Microscope and Density Functional Theory simulations were employed to understand how Co@Pd enhances the properties of Mg/MgH 2 . The improved hydriding/dehydriding kinetics of Mg/MgH 2 are likely closely linked to both the confining impact of c arbon nanotubes and the synergistic interplay of the “spillover” and “hydrogen pump” effects facilitated by the Co@Pd bimetallic catalysts . The excellent hydriding/dehydriding behavior is ascribed to the electron spillover and the phase transformation of Mg 2 Co/Mg 2 CoH 5 and Mg 6 Pd/Pd. These findings offer new insights into the new insights into the rational design of Co@Pd bimetallic catalysts, which are expected to be an optimal solution for supported catalysts in Mg-based solid-state hydrogen storage systems.
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Nanoscale
·
2024
·
IF 5.8
Junqiu Liu,Zhaidong Liu,Chunqin Zhao,Yuting Jiao,Baohong Li,Jiaju Shi,Zichao Chen,Zhen Zhang
Exosomal programmed death ligand-1 (ExoPD-L1) is a vital marker of immune activation in the early stages of tumor therapy and it can inhibit anti-tumor immune responses. However, due to the low expression of ExoPD-L1 in cancer cells, it is difficult to perform highly sensitive assays and accurately differentiate cancer sources. Therefore, we constructed a coaxial dual-path electrochemical biosensor for highly accurate identification and detection of ExoPD-L1 from lung cancer based on chemical–biological coaxial nanomaterials and nucleic acid molecular signal amplification strategies. The measurements showed that the detected ExoPD-L1 concentrations ranged from 6 × 102 particles per mL to 6 × 108 particles per mL, and the detection limit was 310 particles per mL. Compared to other sensors, the electrochemical biosensor designed in this study has a lower detection limit and a wider detection range. Furthermore, we also successfully identified lung cancer-derived ExoPD-L1 by analyzing multiple protein biomarkers expressed on exosomes through the “AND” logic strategy. This sensor platform is expected to realize highly sensitive detection and accurate analysis of multiple sources of ExoPD-L1 and provide ideas for the clinical detection of ExoPD-L1.
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International Journal of Nanomedicine
·
2024
·
IF 6.6
Meng Wei,Xiaobo Wang,Yunhai Mo,Cunqing Kong,Mengqi Zhang,Guanhua Qiu,Zhihong Tang,Jie Chen,Feixiang Wu
Introduction Current therapeutic strategies, including immune checkpoint blockade (ICB), exhibit limited efficacy in treating hepatocellular carcinoma (HCC). Nanoparticles, particularly those that can accumulate specifically within tumors and be activated by sonodynamic therapy (SDT), can induce immunogenic cell death (ICD); however, ICD alone has not achieved satisfactory therapeutic effectiveness. This study investigates whether combining ICB with ICD induced by nanoparticle-mediated SDT could enhance anti-tumor immunity and inhibit HCC growth.Methods We developed an iron-based micelle nanodelivery system encapsulating the Near-Infrared Dye IR-780, which was surface-modified with a cyclic tripeptide composed of arginine-glycine-aspartic acid (cRGD). This led to the synthesis of targeted IR780@FOM-cRGD nanoparticles. These nanoparticles were specifically engineered to kill tumor cells under sonication, activate immunogenic cell death (ICD), and be used in conjunction with immune checkpoint blockade (ICB) for the treatment of hepatocellular carcinoma (HCC).Results The synthesized IR780@FOM-cRGD nanoparticles had an average diameter of 28.23±1.750 nm and a Zeta potential of −23.95±1.926. Confocal microscopy demonstrated that IR780@FOM-cRGD could target HCC cells while minimizing toxicity to healthy cells. Upon sonodynamic activation, these nanoparticles consumed significant amounts of oxygen and generated substantial reactive oxygen species (ROS), effectively killing tumor cells and inhibiting the proliferation, invasion, and migration of H22 cells. Hemolysis assays confirmed the in vivo safety of the nanoparticles, and in vivo fluorescence imaging revealed significant accumulation in tumor tissues. Mouse model experiments showed that combining ICB(which induced by Anti-PD-L1) with ICD (which induced by IR780@FOM-cRGD), could effectively activated anti-tumor immunity and suppressed tumor growth.Discussion This study highlights the potential of IR780@FOM-cRGD nanoparticles to facilitate tumor eradication and immune activation when used in conjunction with Anti-PD-L1 therapy. This combination represents a non-invasive, efficient, and targeted approach for the treatment of hepatocellular carcinoma (HCC). By integrating sonodynamic therapy with immunotherapy, this strategy promises to substantially improve the effectiveness of traditional treatments in combating HCC, offering new avenues for clinical application and therapeutic innovation.
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