APPLIED SURFACE SCIENCE
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2022
·
IF 7.392
Shuqian Xie,Hui Huang,Lu Deng,Junhong Li,Ruirui Yue,Jingkun Xu
Exploration of suitable support materials for noble metal nanocatalysts to reduce the mass loading and optimize the electrocatalytic performance for ethylene glycol oxidation reaction (EGOR) remains a key challenge. Herein the crinkly polypyrrole (PPy)-modified reduced graphene oxide (rGO) was prepared through a facile and efficient in-situ polymerization approach and utilized as the support for Pd nanoparticles . PPy as “spacers” coating on the surface of rGO nanosheets, inhibiting the aggregation and restacking, which greatly increased the available surface area of rGO. Furthermore, this interface-rich structure can offer an efficient pathway for electron conduction, which helps to improve the electrochemical properties of the catalyst. More impressively, the optimized Pd-PPy-rGO 1 nanocomposite outperforms the Pd-PPy and commercial Pd-C with the higher mass activity/specific activity (5550.2 mA mg Pd -1 /30.0 mA cm −2 ), the improved intrinsic activity (TOF value of 6.5 s −1 ) and the enhanced stability toward electrocatalytic EGOR. The superior electrocatalytic performance benefits from the increased specific surface area of the crinkly and interface-rich PPy-rGO and the high utilization efficiency of Pd active sites during the EGOR. This work is expected to give a rational avenue to design interface-rich conducting polymer-rGO nanocomposite support for fuel cells anode catalysts.
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SCIENCE OF THE TOTAL ENVIRONMENT
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2022
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IF 10.753
Xiao-Qiu Lin,Jia-Mei You,Ling-Yu Meng,Naoko Yoshida,Jing-Long Han,Cong-Ju Li,Ai-Jie Wang,Zhi-Ling Li
Tetrabromobisphenol A (TBBPA), a hazardous and persistent flame retardant , has been widely detected in the natural aquatic system. The acceleration of reductive debromination (rate-limiting process) is vital during the decomposition and detoxification of TBBPA. This study achieved superior TBBPA electrochemical reductive debromination performance by nano Pd doped Ni foam electrode (4.8 times higher than Ni foam electrode). The optimal TBBPA reductive debromination performance was obtained under −1.2 V of cathode potential, 1.2 wt% of Pd loading, 10 mg L −1 of TBBPA and 100 mM of Na 2 SO 4 as the electrolyte solution. UPLC-QTOF-MS verified that Br atoms in TBBPA were removed sequentially to form bisphenol A as the major product. Most TBBPA was reductively debrominated by atomic H* through indirect hydrodebromination, evidenced by the atomic H* quenching test. The higher solution conductivity and appropriate TBBPA concentration would contribute to the debromination efficiency. Excessive H 2 generation whether by over negative potential or H atom richness electrolyte largely disturbed the reaction process and restricted the debromination. The improved generation of reductant (H*) ads Pd was the most significant, while excessive Pd loading would make aggregation and limit the debromination efficiency. The study confirmed the optimization strategies of conditions for Pd/Ni foam electrode and revealed the related function mechanism for stimulating TBBPA electrochemical reduction, giving suggestions for the efficient removal of TBBPA in the aquatic environment.
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CHINESE JOURNAL OF CATALYSIS
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2022
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IF 12.92
Zhenyu Li,Liyuan Huai,Panpan Hao,Xi Zhao,Yongzhao Wang,Bingsen Zhang,Chunlin Chen,Jian Zhang
The selective oxidation of 2,5-bis(hydroxymethyl)furan (BHMF) in this work was proven as a promising route to produce 2,5-furandicarboxylic acid (FDCA), an emerging bio-based building-block with wide application. Under ambient pressure, the modified carbon nanotube-supported Pd-based catalysts demonstrate the maximum FDCA yield of 93.0% with a full conversion of BHMF after 60 min at 60 °C, much superior to that of the traditional route using 5-hydroxymethylfurfural (HMF) as substrates (only a yield of 35.7%). The participation of PdH x active species with metallic Pd can be responsible for the encouraging performance. Meanwhile, a possible reaction pathway proceeding through 2,5-diformylfuran (DFF) and 5-formyl-2-furancarboxylic acid (FFCA) as process intermediates is suggested for BHMF route. The present work may provide new opportunities to synthesize other high value-added oxygenates by using BHMF as an alternative feedstock.
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MICROCHIMICA ACTA
·
2022
·Vol. 189
·期 2
·1-10
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IF 6.408
Huang Hui,Xie Shuqian,Deng Lu,Yuan Jie,Yue Ruirui,Xu Jingkun
A nanocomposite of rGO/MXene-Pd/rGO with hierarchical structure based on Ti 3 C 2 T x MXene, Pd nanoparticles, and reduced graphene oxide (rGO) was synthesized by a green approach. Ti 3 C 2 T x MXene decorated with Pd nanoparticles (MXene-Pd) was prepared first. Then, graphene oxide (GO), MXene-Pd, and GO were coated on the surface of the glassy carbon electrode (GCE) in sequence. After each coating of the GO layer, the GO nanosheets were reduced to rGO electrochemically. The fabricated rGO/MXene-Pd/rGO hierarchical framework performs a pie structure with MXene-Pd as the stuffing and rGO nanosheets as the crust, which will be beneficial to the enhancement of its electrochemical sensing performance. As compared with other electrodes, the rGO/MXene-Pd/rGO/GCE exhibited higher electrocatalytic activity and better sensing performance for luteolin detection, with a wide linear range of 6.0 × 10 −10 to 8 × 10 −7 M and 1.0 × 10 −6 to 1.0 × 10 −5 M (oxidation peak potential E pa = 0.34 V vs . SCE), a low detection limit of 2.0 × 10 −10 M, and a high sensitivity of 112.72 µA µM −1 cm −2 . Moreover, the fabricated sensor also showed high selectivity, reproducibility, and repeatability toward the detection of luteolin. The real sample analysis for luteolin in honeysuckle was successfully carried out by rGO/MXene-Pd/rGO and verified with high-performance liquid chromatography (HPLC) analysis techniques with acceptable results. All the above tests indicate the promising application prospect of the rGO/MXene-Pd/rGO framework for luteolin detection in honeysuckle and other herbs containing luteolin. Graphical abstract
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2022
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IF 9.965
Zongtang Liu,Haini Yang,Mian Wang,Yufeng Sun,Zhenghao Fei,Shujuan Chen,Rui Luo,Lin Hu,Chenggang Gu
Effective removal of polybrominated diphenyl ethers (PBDEs) from the environment is essential for the ecosystem and human health. Reductive debromination of PBDEs by nanoscale zerovalent iron (nZVI) has become an important technology. However, the agglomeration and low persistence catalytic activity of nZVI particles have become urgent problems to be improved. Herein, we report the first application of a new organo-attapulgite (OA) supported Fe/Pd nanoparticles (OA-Fe/Pd) composite for decabromodiphenyl ether (BDE209) removal. BDE209 was efficiently removed using OA-Fe/Pd with a reaction rate that was 9.97 times greater than that of the nZVI due to the synergetic effect of support material OA and Pd loading. OA could prevent nZVI particles from agglomeration and adsorb BDE209 molecules to its surface. Pd could supply atomic hydrogen and also prevent the oxidation of nZVI particles. The degradation of BDE209 by OA-Fe/Pd was affected by many factors and followed pseudo first-order kinetics. The degradation of BDE209 by OA-Fe/Pd underwent a stepwise debromination manner with the H-transfer dominant mechanism. BDE209 (25 mg∙L -1 ) could be degraded to penta-BDEs to diphenyl ether (DE) by 3.0 g∙L -1 OA-Fe/Pd within 240 min under neutral condition. This study provides some inspiration for improving the removal efficiency of PBDEs with nZVI-based materials.
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Green Energy & Environment
·
2022
·
IF 12.781
Daqiang Yan,Lin Zhang,Lei Shen,Runyu Hu,Weiping Xiao,Xiaofei Yang
Developing high efficient Pd-based electrocatalysts for oxygen reduction reaction (ORR) is still challenging for alkaline membrane fuel cell, since the strong oxygen adsorption energy and easy agglomerative intrinsic properties. In order to simultaneously solve these problems, Pd/Co 3 O 4 –N–C multidimensional materials with porous structures is designed as the ORR catalysts. In details, the ZIF-67 with polyhedral structure was firstly synthesized and then annealed at high-temperature to prepare the N-doped Co 3 O 4 carbon-based material, which was used to homogeneously confine Pd nanoparticles and obtained the Pd/Co 3 O 4 –N–C series catalysts. The formation of Co–N and C–N bond could provide efficient active sites for ORR. Simultaneously, the strong electronic interaction in the interface between the Pd and N-doped Co 3 O 4 could disperse and avoid the agglomeration of Pd nanoparticles and ensure the exposure of active sites, which is crucial to lower the energy barrier toward ORR and substantially enhance the ORR kinetics. Hence, the Pd/Co 3 O 4 –N–C nanocompounds exhibited excellent ORR catalytic performance, ideal Pd mass activity, and durability in 0.1 mol L −1 KOH solution compared with Co 3 O 4 –N–C and Pd/C. The scalable synthesis method, relatively low cost, and excellent electrochemical ORR performance indicated that the obtained Pd/Co 3 O 4 –N–C electrocatalyst had the potential for application on fuel cells.
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Materials Today Chemistry
·
2022
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IF 7.613
T. Huang,Z. Yu,B. Yuan,L. Jiang,Y. Liu,X. Sun,P. Liu,W. Jiang,J. Tang
The presence of bacteria, existing as highly organized biofilm communities, in chronic non-healing wounds has been identified as a significant impediment for wound healing. Nanozymes , with unique antimicrobial mechanisms, as a new alternative for antibiotics, have the potential to synergize with nitric oxide (NO) with enhanced antibacterial and antibiofilm ability. However, the always-on state of nanozymes and the reactivity of NO limit their clinical applications. In this context, an intelligent and multifunctional Pd-MOF@PAzo@SNP nanoplatform was fabricated using UiO-66 as a palladium (Pd) nanozyme-loading vehicle, then a surface modification with photosensitive polyazobenzene (PAzo), and the adsorption of the NO donor sodium nitroprusside (SNP) via a host-guest interaction between β -cyclodextrin-modified hyaluronic acid ( β -CD-HA) and azobenzene. The activity of Pd-nanozyme was easily controlled via ultraviolet (UV) light, and its photosensitivity was regulated by changing the side-chain unit length of PAzo. Furthermore, NO was released in response to the UV irradiation and played a synergistic role with the peroxidase activity of Pd nanozyme, exhibiting excellent antibacterial and antibiofilm activity in the presence of 0.01 mM hydrogen peroxide (H 2 O 2 ). In vivo , Pd-MOF@PAzo@SNP accelerated the healing of a biofilm-infected diabetic wound by dispersing the biofilm, reducing bacterial burden, and promoting angiogenesis and collagen deposition. Overall, the nanoplatform provides a reliable and highly efficient strategy to develop an intelligent nanozyme synergy with NO therapy in chronic wound management.
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Catalysis Science & Technology
·
2022
·Vol. 12
·期 6
·1788-1798
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IF 6.177
Jing Zhao,Yanzhuo Zhang,Hucheng Zhang,Haiyan Wang,Jianji Wang
Hydrogen spillover is an important theme for hydrogen storage and H-involving catalytic reactions. This work shows that catalytic reactivity and selectivity can be revealed by differentiating the energetic characteristics of spilled H species. With the assistance of Ti, F and C in MXenes, Pd1.8Ni@Ti3C2Tx presents a high capacity for spillover hydrogen storage at ambient temperatures, and the rich oxygenated groups act as the main carriers of hydrogen spillover around metal nanoparticles. Thermodynamic analysis reveals that the catalytic performances are energetically dominated by the adsorption enthalpies of the active spilled H species rather than the amount of spillover hydrogen, and can be tuned by alloying and surface modification. The ideas are verified from the excellent catalysis, chemoselectivity and stereoselectivity of Pd1.8Ni@Ti3C2Tx in semihydrogenations. The strategy of maximizing catalytic performances is applicable to other Pd-based bimetals@Ti3C2Tx, such as Pd2.6Co@Ti3C2Tx and Pd1.5Fe@Ti3C2Tx, and provides new energetics perspectives to understand the catalytic mechanism in spillover-involving chemical procedures.
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Molecular Catalysis
·
2021
·
IF 5.062
Jing Zhao,Hucheng Zhang,Haiyan Wang,Jianji Wang
A highly attractive aim is to turn CO 2 into useful chemicals selectively and efficiently, but it still retains great challenging to understand the relations between catalytic performances and interface properties. Here, we report an alternative solution to relate the catalytic activity with the strengths of Lewis acids and bases on the Pd-CoO x interfaces. CoO∙TiO 2 /TiO 2 and CoO x /TiO 2 possess the wide spectrum of Lewis acid/base centres, and give the low selectivity and conversion. The introduction of Pd can focus them on the intrinsic centres, and makes Pd-CoO∙TiO 2 /TiO 2 and Pd-CoO x /TiO 2 represent the ideal catalysis. With temperature-programmed desorptions of CO 2 , CO and NH 3 , it is evidenced that the catalytic hydrogenations of CO 2 to CO, CH 4 and CH 3 OH depend on the cooperation of the Lewis acidic/alkaline centres on the interfaces. The studies provide guidelines for rational design and synthesis of heterogeneous catalysts including but not limited to CO 2 hydrogenation.
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JOURNAL OF APPLIED PHYSICS
·
2023
·Vol. 134
·期 8
·
IF 3.2
Li Gaojie,Zhang Linqi,Du Kai,Wang Xinxin,Yin Menghao
Reducing the working temperature and increasing sensitivity and selectivity has always been a research hotspot in the field of MOS based gas sensors. In this work, improved triethylamine (TEA) sensing performance and mechanism of SnO 2 by doping Pd have been investigated. SnO 2 nanoparticles and Pd-SnO 2 with different doping amounts of Pd (0%, 0.1%, 0.3%, 0.5%, and 0.7%) were successfully prepared by the hydrothermal method. The size of SnO 2 nanoparticles is very uniform (∼15 nm). The SnO 2 sensor exhibited the highest sensitivity to ethanol at 290 °C. After Pd doping, Pd/SnO 2 sensors not only reduced the optimum working temperature but transformed selectivity from ethanol to TEA. In the Pd-SnO 2 system, the 0.5Pd-SnO 2 sensor exhibited high sensitivity (61), fast response-recovery properties (16 s/6 s) to 50 ppm TEA, lower detection limits (0.1 ppm), good repeatability, and higher selectivity. Furthermore, based on density functional theory calculations, the improved TEA sensing performance of 0.5Pd-SnO 2 sensors can be attributed to the improved surface activity of SnO 2 by Pd doping and the catalytic activation of O 2 and TEA by Pd.
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ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Di Chuan,Rangrang Fan,Bo Chen,Yangmei Ren,Min Mu,Haifeng Chen,Bingwen Zou,Haohao Dong,Aiping Tong,Gang Guo
In developing countries, the incidence of colorectal cancer (CRC) is on the rise. The combination of programmed cell death ligand-1 (PD-L1) siRNA (siPD-L1) and mild photothermal therapy (PTT) is a promising strategy for CRC treatment. In this study, dopamine-modified polyethylenimine (PEI) was prepared to fabricate an IR780 and siPD-L1 codelivery lipid–polymer hybrid nanoparticle (lip@PSD-siP) for the photothermal immunotherapy of CRC. The modification of dopamine can significantly reduce the cytotoxicity of PEI. lip@PSD-siP can be effectively taken up by CT26 cells and successfully escaped from lysosomes after entering the cells for 4 h. After CT26 cells were transfected with lip@PSD-siP, the PD-L1 positive cell rate decreased by 82.4%, and its PD-L1 knockdown effect was significantly stronger than the positive control Lipo3000-siP. In vivo studies showed that lip@PSD-siP-mediated mild PTT and efficient PD-L1 knockdown exhibited primary and distal tumor inhibition, metastasis delay, and rechallenged tumor inhibition. The treatment with lip@PSD-siP significantly promoted the maturation of dendritic cells in lymph nodes. The amount of T cell infiltration in the tumor tissues increased significantly, and the frequency of CD8+ T cells and CD4+ T cells was significantly higher than that of other groups. The percentage of immunosuppressive regulatory cells (Tregs) in the tumor tissue on the treatment side decreased by 88% compared to the PBS group, and the proportion of CD8+CD69+ T cells in the distal tumor tissue was 2.8 times that of the PBS group. The memory T cells of mice in the long-term antitumor model were analyzed. The results showed that after treatment with lip@PSD-siP, the frequency of effector memory T cells (Tem cells) significantly increased, suggesting the formation of immune memory.
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ACS Applied Nano Materials
·
2023
·
IF 5.9
Jinwu Hu,Ran Li,Xin Wang,Shaozhen Wang,Caihong Fang
Constructing an appealing architecture is of great significance to improving the electrocatalytic activity and stability of Pt-based nanocatalysts. In this work, we successfully synthesized porous Pd@PdPt core/shell nanocrystals via a facile one-pot method, which possess several architectural and compositional advantages, involving porous outer, ultrathin branches, an open mesoporous skeleton, a core/shell structure, and an alloyed composition. These morphological features and the synergistic effect between different components in the alloy endow the Pd@PdPt nanostructures with abundant active sites, effective mass transfer, strain in the particle, and the electronic coupling effect. The Pd@PdPt nanoalloy therefore exhibits excellent electrocatalytic performances in alcohol oxidation reactions. Impressively, the Pd5Pt4 nanocubes exhibit a higher mass/specific activity of 3.225 A mgPt+Pd–1/34.49 A m–2 for the ethanol oxidation reaction, which is even 4.00-/2.39-fold as high as that of commercial Pt/C. Moreover, the Pd5Pt4 nanocubes also show a superior mass activity of 2.824 A mgPt+Pd–1/37.66 A m–2 toward the methanol oxidation reaction, which is up to 4.20/2.40 times that of the commercial Pt/C. The Pd@PdPt also has enhanced electrocatalytic stability. More importantly, the porous Pt5Pd4 nanocubes still demonstrate superior electrocatalytic activities of 0.259, 1.19, 2.65, and 2.76 A mgPt+Pd–1 for the oxidation of glucose, isopropyl alcohol, glycerol, and ethylene glycol, respectively. We therefore believe that these universal electrocatalysts have the potential to promote practical applications in fuel cells.
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