CHEMICAL ENGINEERING JOURNAL
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2018
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IF 6.735
Tianyu Guo,Xiaorong Nie,Jianping Du,Jinping Li
Methane oxidation is a strong exothermal reaction, the heat released from which can be utilized and the greenhouse effect caused by emitted methane, particularly low-concentration methane (LCM), can be further relieved. Presently, one of the key problems is to develop an efficient catalyst material for promoting LCM oxidation. Here, we synthesized an alumina with 2D feather-like lamella structure (FLAO), which is suitable for industrial applications. The samples were characterized by X-ray diffraction, scanning/transmission electron microscopy, X-ray photoelectron spectroscopy and nitrogen adsorption/desorption techniques. The results show that as-synthesized alumina has feather-shaped morphology and 2D slices structures, which form loose framework. Pd nanoparticles were easy to be anchored and well-dispersed on the surface of alumina. The FLAO-supported Pd catalysts exhibited high activity and stability. For 360000 mL g −1 h −1 space velocity, the LCM conversion research above 90% at 400 °C, and only decrease 8.6% after 50 h reaction at 450 °C, suggesting that as-synthesized 2D alumina slice has potential application for highly efficient removal of low-concentration methane from ventilation air.
研究领域:
材料科学
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环境科学
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JOURNAL OF NANOBIOTECHNOLOGY
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2026
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IF 15
Zhao Mengfei,Zhang Jichuan,Guan Meng,Li Xuanhan,Sun Huating,Mao Kuirong,Tan Huizhu,Zhang Yijia,Meng Xandi,Cong Xiuxiu,Xin Yanbao,Wang Haorui,Yu MeiLing,Chen Si,Zhou Hongxv,Wang Xinhe,Yang Yong-Guang,Sun Tianmeng,Zhang Yuning
Immune checkpoint blockade (ICB) remains limited by the immunosuppressive tumor microenvironment (TME) and by the difficulty of coordinating therapeutic agents that act in distinct tumor compartments. In particular, checkpoint antibodies must function in the tumor stroma, whereas TME-remodeling small molecules often require intracellular access, creating an extracellular–intracellular delivery mismatch that conventional carriers rarely resolve. Here, we develop an acid-gated, esterase-amplified AND-gated dendritic nanogel (DNG) for the spatiotemporally sequential codelivery of anti-PD-1 antibody (aPD-1) and the PPARδ antagonist GSK3787. The DNG comprises a PEG corona for reversible aPD-1 adsorption and a hydrophobic dendritic core for GSK3787 encapsulation. Under the combined cues of tumor acidity and esterase activity, the nanogel undergoes progressive dissociation, triggering preferential extracellular release of aPD-1 in the tumor stroma, followed by tumor-cell internalization of the GSK3787-loaded core for intracellular drug action. This AND-gated design enables spatially resolved pharmacology rather than simple codelivery. In a melanoma model, DNG@(GSK3787 + aPD-1) markedly enhances antitumor efficacy, thereby promotes CD8⁺ T cell infiltration, and elicits systemic antitumor immune responses. Mechanistically, we identify a tumor cell-centric mode of immune remodeling and further show that the dendritic core actively governs not only small-molecule encapsulation, but also antibody retention and triggered release. Together, this work establishes a materials strategy for overcoming extracellular–intracellular delivery mismatch in combination immunotherapy. Graphical AND-gated dual-responsive nanogel enables spatiotemporally sequential extracellular delivery of aPD-1 and intracellular delivery of GSK3787, thereby overcoming the extracellular–intracellular delivery mismatch and synergistically remodeling the tumor immune microenvironment for enhanced cancer immunotherapy.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2021
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IF 8.128
Xingchi Li,Huaming You,Cheng Wang,Dongmei Liu,Rui Yu,Siyu Guo,Yuan Wang,Yukou Du
Modifying the electronic structure and optimizing the geometric structure can expeditiously tune the electrocatalytic properties of catalysts, resulting in considerably enhanced electrocatalytic performance towards electrocatalytic oxidation of liquid fuels . We herein report a simple synthetic strategy to prepare Bi-doped 3D taraxacum-like Pd nanocages (NCs) composed of porous nanosheets , which possess high surface areas and strong synergistic effects. Notably, a trace of Bi diffuses into the lattice of Pd and increases the electronic effects of the surface of Pd, endowing PdBi-0.5 NCs/C with superior electrocatalytic performance towards ethanol oxidation reaction (EOR). The mass activity and specific activity of PdBi-0.5 NCs/C were 3494.8 mA mg Pd −1 and 10.37 mA cm −2 , being 4.08- and 4.82- fold enhancements as compared with commercial Pd/C, respectively. Moreover, the highly open porous 3D nanocages structure with rich active sites and defects can also facilitate the mass/electron transfer to favor the EOR kinetics.
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PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2021
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IF 13.273
Jiasheng Zhou,Zimo Lou,Zheni Wang,Chuchen Zhou,Cheng Li,Shams Ali Baig,Xinhua Xu
The CTAB-Pd/GAC catalyst was obtained by functionalizing palladium/granular activated carbon (Pd/GAC) with cetyltrimethylammonium bromide (CTAB), which was used for the electrocatalytic reductive dechlorination of 2,4-dichlorobenzoic acid (2,4-DCBA). The degradation rate of 2,4-DCBA by 40 mg g −1 CTAB-Pd/GAC was 9.8 × 10 −3 (min −1 g −1 Pd), which was 11 folds than that by Pd/GAC (0.9 × 10 −3 min −1 g −1 Pd), and the value of q e, 2,4-DCBA / q e, BA was 2.33 as compared to 0.67 for Pd/GAC. The combined result of dechlorination and adsorption experiments suggested that the functionalization by CTAB would enhance the 2,4-DCBA concentration on the surface of CTAB-Pd/GAC, and accelerate the degradation rate. However, the removal efficiency of 2,4-DCBA would decrease when the CTAB load reached 80 mg g −1 , due to the excessive adsorption capacity for dechlorinated product. Density functional theory (DFT) calculations also proved that CTAB would increase adsorption capacity of catalyst and selective adsorption behavior of 2,4-DCBA, which accelerated the degradation rate of 2,4-DCBA.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2021
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IF 19.503
Xiaoli Li,Ting Wang,Ziqiang Zheng,Qing Yang,Can Li,Benxia Li
Developing photocatalysts for coproduction of hydrogen fuel and valuable chemicals is highly desired but still challenging. Herein, Pd-modified defective HNb 3 O 8 photocatalyst (denote as Pd/HNb 3 O 8 -H 2 ) consisting of dispersive Pd sites and abundant surface oxygen vacancies (V O s) was prepared via the thermal treatment of Pd 2+ -incorporated HNb 3 O 8 in H 2 /Ar gas. The existence of Pd favors the formation of V O s on HNb 3 O 8 , enabling the synchronous construction of Pd and V O dual active sites. The spectroscopy and photoelectrochemical studies demonstrate the advantages of Pd/HNb 3 O 8 -H 2 photocatalyst in promoting the separation and migration of photoinduced charge carries. The Pd/HNb 3 O 8 -H 2 photocatalyst exhibits the outstanding performance toward photocatalytic proton reduction coupled with selective benzyl-alcohol oxidation , achieving the optimal production rates of H 2 and benzaldehyde as high as 3.17 and 2.76 mmol·g cat −1 h −1 , respectively. The experimental and theoretical investigations have expounded the synergistic mechanism of Pd and V O dual active sites in boosting photocatalytic coproduction of H 2 and benzaldehyde.
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Molecular Catalysis
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2020
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IF 3.687
Qian Wang,Meiling Ge,Yuheng Dou,Fu Yang,Junkai Wang,Yuyang Shao,Agen Huang
Polymer supports play an important role in noble metal loaded catalysts. In this study, palladium clusters stabilized by several polyamides have been widely studied in the oxidation of benzyl alcohol under airflow. The different kinds of polyamides (PADs) were synthesized with aromatic diamines and trimesoyl chloride by mechanical grinding method and solvent-heat method. Polyamide support was synthesized through mechanical grinding method. And the laminar structure and abundant amide bonds of polyamide can help obtain ultrafine Pd clusters with a mean particle size of 1.76 nm. The Pd 0.5 @PAD-2-M effectively catalyzed benzyl alcohol into benzaldehyde with a conversion of 96.1 % and turnover number (TON) of 1441 under 90 °C in water which was 2.5 times higher than the commercial Pd/C catalyst. High TON value of 6505 was also achieved in solvent-free system. This work reveals the advantages of laminar structure of polyamide in dispersing Pd clusters and promoting benzyl alcohol conversion. Besides, the carrier properties of amphipathy and substrate adsorption were also investigated to illustrate the significance of interfacial effect for laminar catalyst in heterogeneous catalysis.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2020
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IF 4.65
Kelin Hu,Feipeng Wang,Zijia Shen,Hongcheng Liu,Jianglin Xiong
In this paper, Pd/ZnO–SnO 2 hollow nanofibers prepared by electrospinning and magnetron sputtering . The sensing materials exhibited extraordinary hydrogen (H 2 ) sensing behavior – the response reached 171 at 270 °C, and besides, the response time and recovery time were as low as 19 s and less than 1 s at 240 °C, with steady high selectivity and good repeatability. Such an enhanced sensing performance could be attributed to the Pd/ZnO/SnO 2 ternary heterojunctions formed in the hollow nanofibers. Moreover, the materials were studied by X-ray diffraction (XRD), energy dispersive X-ray spectroscopy (EDS), X-ray photoelectron spectroscopy (XPS), transmission electron microscopy (TEM) and especially the morphology formation process was further explained. The existence of Pd was confirmed to increase the resistance modulation range of heterojunction. In addition, the gas sensing mechanism based on the structure was proposed.
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Nanoscale
·
2020
·Vol. 13
·期 6
·3528-3542
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IF 6.895
Yaxing Liu,Weiyin Li,Guizhe Zhao,Gang Qin,Yuexia Li,Yaqing Liu
The lack of direct insight into the microstructural evolution of catalytic materials under electrochemical polarization has inhibited the development of heterogeneous catalysts. By investigating a typical Au@Pd core–shell nanostructure, the present study discloses the microstructural evolution of heterogeneous catalytic materials during the methanol electrooxidation reaction (MOR). The electrocatalytic activity of the as-prepared Au@Pd_core–shell nanoparticles continuously increased during the first 100 successive voltammetry cycles of the MOR. Microstructural characterization studies revealed that during the MOR, an Au/Pd mixed bimetallic shell was formed by the self-driven microstructural evolution of the Au@Pd_core–shell nanoparticles. Both the experimental and calculation results indicated that the Au/Pd mixed bimetallic shell reduced the binding strength of OH− and CO on the catalyst surface. The exposed Au atoms in the shell region also produced large-scale reactive ˙OH radicals that facilitated the oxidative removal of the adsorbed carbonaceous species from the adjacent Pd active sites.
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高影响因子
ACS Catalysis
·
2020
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IF 12.35
Zhongjie Cai,Jiajun Dai,Wen Li,Kok Bing Tan,Zhongliang Huang,Guowu Zhan,Jiale Huang,Qingbiao Li
Utilization of CO2 and its conversion to value-added chemicals are highly desirable to alleviate the environmental concerns caused by the massive anthropogenic CO2 emission. Although In2O3/Pd have been employed as efficient catalysts for hydrogenation of CO2 to methanol, the electronic effects by strong metal–support interaction (SMSI) between Pd and In2O3 are poorly understood, which is greatly affected by the morphology of In2O3. Herein, we use MIL-68(In) nanorod as a morphological template for the synthesis of hollow In2O3 nanotubes (h-In2O3) and the preparation of supported Pd catalysts for CO2 hydrogenation to methanol. Interestingly, loading Pd on h-In2O3 showed a much higher performance than In2O3 with other morphologies, which exhibited almost unchanged CO2 conversion of 10.5%, methanol selectively of 72.4%, and methanol space-time yield of 0.53 gMeOH h–1 gcat–1 over 100 h on stream at 3 MPa and 295 °C. After in-depth characterizations, we found that the different electronic properties of Pd species on In2O3 can be finely tuned by diverse synthetic conditions, which were responsible for high activity and stability. The molar fraction of Pd2+ species in the h-In2O3/Pd catalyst reached 67.6%, 3.2 times that of the In2O3@Pd catalyst (21.3%), due to the different surface chemistry of In2O3. Density function theory results indicated that the Pd donated more electrons to the curved In2O3 (222) surface than the pristine surface, and Pd2+ was critical to facilitate H2 adsorption and formation of the surface oxygen vacancy. This work demonstrates that controlling the morphology of In2O3 can modify both the Pd electronic property and SMSI between Pd and In2O3, which are the origins of the high catalytic performance.
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ACS Sustainable Chemistry & Engineering
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2020
·
IF 7.632
Hao Huang,Rui Zong,Hao Li
This work reports an innovative route for biomass upgrading via hydrodeoxygenation (HDO) reactions which avoids external high-pressure hydrogen supply and harsh conditions (such as high-temperature or additives). A novel Pd/CFR catalyst with controllable oxygen groups and defects was synthesized with low-load Pd supported on resorcinol–formaldehyde resin carbon spheres (CFR) for selective hydrodeoxygenation of vanillin under mild conditions. The as-prepared Pd/CFR-800 catalyst shows excellent activity (>99.5% yield of 2-methoxy-4-methylphenol) using polymethylhydrosiloxane (PMHS) as green hydride source within 1 h at 70 °C, in the absence of additives. According to spectral analyses, the concentration of carbon skeleton defects and hydroxyl functional groups on the catalyst can be adjusted by the carbonization temperature. Combined with experimental results and mechanistic studies, the synergistic effect of hydroxyl groups and adjacent defects was deemed as the main reason for the strong adsorption of the substrate, which significantly facilitated the key hydrogenolysis step. Furthermore, the as-prepared Pd/CFR-800 catalyst has shown excellent recyclability after used for five times. The in situ regulation of functional groups and defects on carbon materials provides new ideas for designing high-performance catalysts for the catalytic transformation of various lignin derivatives.
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ACS Sustainable Chemistry & Engineering
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2020
·
IF 7.632
Wen Li,Kuncan Wang,Guowu Zhan,Jiale Huang,Qingbiao Li
The chemical transformation of CO2 to value-added chemicals and fuels remains a daunting research challenge, requiring the development of more efficient catalysts. The present work offers highly active integrated nanocatalysts for CO2 hydrogenation to dimethyl ether (DME) through tandem catalysis, that is, Pd/ZnO converts CO2 to methanol, and bio-ZSM-5 further catalyzes methanol dehydration to DME. Notably, the hierarchically porous bio-ZSM-5 with high pore connectivity was prepared by using low-cost rice husk and luffa sponge as biotemplates. The formation of bio-ZSM-5 involved three consecutive steps, including (i) diffusion of precursor species, (ii) confined crystal growth, and (iii) calcination treatment to remove the residual biomass. Interestingly, the obtained bio-ZSM-5 possesses abundant hierarchical porosity, including the intrinsic micropores from ZSM-5 frameworks, the mesopores from intracrystalline void space or pinholes in the intergrown zeolite layers, and the macroscopic channels from the original biomass architecture. It was found that the tetrapropylammonium hydroxide amount and Si/Al ratio were two critical factors affecting the crystallinity and porosity of the bio-ZSM-5. The silicon content in biomass (8.3 wt % in rice husk and 0.016 wt % in luffa sponge) also played a crucial role in the synthesis of bio-ZSM-5. Different spatial configurations of Pd/ZnO and bio-ZSM-5 significantly affected the DME yield, wherein spatial distances between the bio-ZSM-5 and Pd/ZnO components were adjusted by controlling the size of Pd/ZnO or the integration manners. The current results indicated that the closest proximity of the bifunctional catalyst was unfavorable for DME production (selectivity < 3%), because of which low-valent Zn cations from Pd/ZnO could displace the Brønsted acid sites on bio-ZSM-5 by ion exchange, and the powder mixing in the mortar was the best combination configuration of Pd/ZnO and bio-ZSM-5, promoting the CO2 conversion (10.8%) with a DME selectivity of 31% under the reaction of 300 °C and 30 bar. Furthermore, as compared to the traditional ZSM-5 based catalyst, the obtained Pd/ZnO/bio-ZSM-5 bifunctional catalysts showed excellent long-term stability in 60 h on stream with a less amount of coke formed in the spent catalysts.
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Molecular Catalysis
·
2020
·
IF 3.687
Ning Xiang,Xiaojin Han,Yarong Bai,Qiaoyan Li,Jianfeng Zheng,Yulin Li,Yaqin Hou,Zhanggen Huang
Supported noble metal catalysts have been widely utilized for HCHO catalytic oxidation. When the active components are fixed, the altering and regulation of the supports would have a huge effect on catalytic performance. Here, two types of Pd/γ-Al 2 O 3 catalysts with different support size (micro-γ-Al 2 O 3 and nano-γ-Al 2 O 3 , respectively) were fabricated and used for HCHO oxidation. Compared with the micro-sized counterpart, the Pd/nano-γ-Al 2 O 3 catalyst exhibited much superior HCHO oxidation performance which could totally oxidize 160 ppm of HCHO into harmless CO 2 under a WHSV of 100,000 mL g cat −1 h −1 at room temperature. Multiple characterizations including XRD, BET, TEM, CO chemisorption, FT-IR, O 2 -TPD, XPS and in situ DRIFTS were implemented to study the effect of γ-Al 2 O 3 support size on physicochemical properties of Pd/γ-Al 2 O 3 catalysts and elucidate the structure-activity relationship. The results revealed that large specific surface area, rich surface OH groups as well as high curvature of nano-γ-Al 2 O 3 not only facilitated HCHO adsorption, but also stabilized highly dispersed Pd species which then promoted the activation of oxygen and boosted formate species decomposition, and consequently leading to the enhanced HCHO oxidation performance of Pd/nano-γ-Al 2 O 3 . This work deepens the comprehension of support size-dependent activity of Pd/γ-Al 2 O 3 catalysts for HCHO oxidation and provides an alternative method to prepare high-performance Pd catalysts for HCHO oxidation.
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