CHEMICAL ENGINEERING JOURNAL
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2022
·
IF 16.744
Yabing Gan,Guoxing Yin,Zhaomin Xu,Huyang Zhou,Ting Yu,Haitao Li,Peng Yin
Gold (Au) and palladium (Pd) species have been widely used in synthetic chemistry, biology, and environmental sciences, raising hard-to-ignore health and environment risks due to their potential toxicity. Herein, a novel dual-functional fluorescent probe was rationally designed and developed for simultaneous quantification and visualization of Au 3+ and Pd species in the environmental and biological systems. Significant fluorescence enhancement at 484 and 606 nm and color changes were observed upon addition of Au 3+ and Pd 0 with high sensitivity. The detection limit for Au 3+ and Pd 0 was as low as 68 nM and 7 nM, respectively. Combined with smartphone chromaticity and dual-channel fluorescence imaging analysis, this probe was successfully applied to the quantification and visualization of Au 3+ and Pd species in real water samples. Thus, simultaneous naked-eye visualization and quantification of Au 3+ and Pd 0 in real water samples was achieved using this probe. The probe was also successfully applied to fluorescence imaging of Au 3+ and Pd 0 in HeLa cells and zebrafish, promoting the monitor and understanding about gold and palladium species in environmental and biological systems.
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高影响因子
FUEL
·
2022
·
IF 8.035
Baicheng Feng,Zichen Zhang,Jiaqiang Wang,Donglin Yang,Qun Li,Yaping Liu,Hengjun Gai,Tingting Huang,Hongbing Song
The catalytic hydrogenation of carbon dioxide (CO 2 ) into formic acid is among the most important reactions to alleviate global warming and realize the carbon cycle. How to achieve rapid activation of CO 2 remains a challenge. In this work, we designed two novel hydrophobic poly(ionic liquid)s (PILs) with a good affinity for CO 2 . Since the abundant N atoms in the PILs can anchor palladium (Pd) nanoparticles, the designed catalyst can rapidly activate CO 2 and H 2 simultaneously, thus efficiently catalyzing the hydrogenation of CO 2 to formic acid under mild conditions. Due to the synergy from the bis(trifluoromethanesulfonyl)amide anion ([Tf 2 N − ]) with strong hydrophobicity and CO 2 affinity and trimethylamine (NEt 3 ) as a low dissociation energy alkaline additive, the resultant Pd/PIL-bip-Tf 2 N exhibited the best catalytic performance on the hydrogenation of CO 2 to formic acid. The TOF value reached 1,190 h −1 in the aqueous solution of NEt 3 at 100 °C, 1 h, and a total pressure of 4 MPa. The activation energy and dissociation energy during the catalytic process were calculated by DFT, indicating that the synergistic effect of NEt 3 is better than that of other alkaline additives. In addition, the catalytic activity of the catalyst remained stable after several cycling experiments. Based on the obtained results, we proposed a possible reaction pathway. Therefore, PILs have great potential as catalyst carrier material for CO 2 hydrogenation.
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JOURNAL OF NANOBIOTECHNOLOGY
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2022
·Vol. 20
·期 1
·1-17
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IF 9.429
Lu Yuan-Fei,Zhou Jia-Ping,Zhou Qiao-Mei,Yang Xiao-Yan,Wang Xiao-Jie,Yu Jie-Ni,Zhang Jin-Guo,Du Yong-Zhong,Yu Ri-Sheng
Background The efficacy of immune checkpoint blockade (ICB), in the treatment of hepatocellular carcinoma (HCC), is limited due to low levels of tumor-infiltrating T lymphocytes and deficient checkpoint blockade in this immunologically "cool" tumor. Thus, combination approaches are needed to increase the response rates of ICB and induce synergistic antitumor immunity.Methods Herein, we designed a pH-sensitive multifunctional nanoplatform based on layered double hydroxides (LDHs) loaded with siRNA to block the intracellular immune checkpoint NR2F6, together with the asynchronous blockade surface receptor PD-L1 to induce strong synergistic antitumor immunity. Moreover, photothermal therapy (PTT) generated by LDHs after laser irradiation modified an immunologically “cold” microenvironment to potentiate Nr2f6-siRNA and anti-PD-L1 immunotherapy. Flow cytometry was performed to assess the immune responses initiated by the multifunctional nanoplatform.Results Under the slightly acidic tumor extracellular environment, PEG detached and the re-exposed positively charged LDHs enhanced tumor accumulation and cell uptake. The accumulated siRNA suppressed the signal of dual protumor activity in both immune and H22 tumor cells by silencing the NR2F6 gene, which further reduced the tumor burden and enhanced systemic antitumor immunity. The responses include enhanced tumor infiltration by CD4+ helper T cells, CD8+ cytotoxic T cells, and mature dendritic cells; the significantly decreased level of immune suppressed regulator T cells. The therapeutic responses were also attributed to the production of IL-2, IFN-γ, and TNF-α. The prepared nanoparticles also exhibited potential magnetic resonance imaging (MRI) ability, which could serve to guide synergistic immunotherapy treatment.Conclusion sIn summary, the three combinations of PTT, NR2F6 gene ablation and anti-PD-L1 can promote a synergistic immune response to inhibit the progression of primary HCC tumors and prevent metastasis. This study can be considered a proof-of-concept for the targeting of surface and intracellular immune checkpoints to supplement the existing HCC immunotherapy treatments.
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PubMed
高影响因子
Journal of Pharmaceutical Analysis
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2022
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IF 14.026
Yinfei Chen,Shiyu Zhu,Jiayu Fu,Jianguo Lin,Yan Sun,Gaochao Lv,Minhao Xie,Tao Xu,Ling Qiu
Despite advances in immunotherapy for the treatment of cancers, not all patients can benefit from programmed cell death ligand 1 (PD-L1) immune checkpoint blockade therapy. Anti-PD-L1 therapeutic effects reportedly correlate with the PD-L1 expression level; hence, accurate detection of PD-L1 expression can guide immunotherapy to achieve better therapeutic effects. Therefore, based on the high affinity antibody Nb109, a new site-specifically radiolabeled tracer, 68 Ga-NODA-cysteine, aspartic acid, and valine (CDV)-Nb109, was designed and synthesized to accurately monitor PD-L1 expression. The tracer 68 Ga-NODA-CDV-Nb109 was obtained using a site-specific conjugation strategy with a radiochemical yield of about 95% and radiochemical purity of 97%. It showed high affinity for PD-L1 with a dissociation constant of 12.34 ± 1.65 nM. Both the cell uptake assay and positron emission tomography (PET) imaging revealed higher tracer uptake in PD-L1-positive A375-hPD-L1 and U87 tumor cells than in PD-L1-negative A375 tumor cells. Meanwhile, dynamic PET imaging of a NCI-H1299 xenograft indicated that doxorubicin could upregulate PD-L1 expression, allowing timely interventional immunotherapy. In conclusion, this tracer could sensitively and dynamically monitor changes in PD-L1 expression levels in different cancers and help screen patients who can benefit from anti-PD-L1 immunotherapy.
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PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Liuxuan Luo,Zehao Tan,Cehuang Fu,Rui Xue,Xiaojing Cheng,Tianzi Bi,Lutian Zhao,Yangge Guo,Xiyang Cai,Jiewei Yin,Shuiyun Shen,Junliang Zhang
Increasing the accessible active sites and especially improving the intrinsic activity are two major effective strategies for enhancing the electrocatalytic activity of nanomaterials. Accordingly, through the trioctylphosphine (TOP)-based CO-assisted solvothermal method and the small-amount Pt 2+ galvanic replacement, highly uniform Pd nanotetrahedrons (NTs) with Pt-doped surfaces are synthesized and supported onto carbon black. Comprehensive experimental and theoretical analyses reveal that, owing to the Pt surface-doped (SD) nanostructure, the conformal formation of surface Pt {111} facets, as well as the strain and electronic effects induced by the Pd–Pt alloy structure, Pd/ SD Pt NTs/C exhibits much better electrocatalytic performance than Pd NTs/C, commercial Pd/C, and Pt/C toward both oxygen reduction and formic acid oxidation reactions, showing greatly improved metal utilization and area/mass-specific activity. This study develops a high-performance bifunctional electrocatalyst, and firstly introduces TOP as the easy-removable surface-energy adjuster for the Pd shape-controlled synthesis, which may be further expanded to other metals and shapes.
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APPLIED ORGANOMETALLIC CHEMISTRY
·
2021
·Vol. 36
·期 3
·e6556
·
IF 4.105
Wen-Jing Qiu,Ming-Wu Gao,Qi Chen,Ao Zheng,Yi-Jia Shi,Xin Liu,Juan-Hong Li,Guo-Liang Dai,Yang Hu,Zi-Xia Lin
Under normal temperature and pressure, a novel improved Fenton system that was named MHACF-MOF-808(Zr) was constructed after the introduction of Pd/MOF-808(Zr) and H 2 to solve the inherent problem of the production of iron sludge in the classic Fenton system. Only trace amount of Fe II was required during the whole reaction because Fe III could be rapidly reduced by the active hydrogen derived from the adsorption and activation of H 2 on the surface of Pd/MOF-808(Zr) composite. The concentration of Fe II could be maintained more than 10 μM. The removal of target pollutant sulfamethazine in this system was mainly relied on the degradation of ·OH verified by both of the direct detection and indirect inhibition (using methanol). By using the calculation of Laplacian bond order, the degradation pathway of sulfamethazine followed by the cleavage of N S bond. This prediction was verified by the detection of intermediate products. Only 21% sulfamethazine could be degraded after 3-h reaction in the classic Fenton reaction system, while it could be thoroughly degraded in 1.5 h in the MHACF-MOF-808(Zr) system. The influence of main parameters on the degradation effect of sulfamethazine, such as initial pH, the flow of H 2 , dosage of Pd/MOF-808(Zr), concentration of sulfamethazine, ferrous, and hydrogen peroxide, were systematically studied. Based on the relative stability of Pd/MOF-808(Zr) confirmed by the morphological characterization, sulfamethazine could be efficiently degraded in the MHACF-MOF-808(Zr) system.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2021
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IF 13.273
Yuan Shu,Xiaolan Duan,Qiang Niu,Rongyong Xie,Pengfei Zhang,Yunxiang Pan,Zifeng Ma
Zinc oxide is a key material in catalysis. Designing of ZnO crystal aggregates with the surface defect has received significant attention. Herein, we synthesized ZnO aggregates with tiny primary nanoparticles through a mechanochemistry-assisted salt-templating (potassium chloride) method. Interestingly, this KCl-templating strategy could lead to significant increase in specific surface area (SSA) of ZnO (up to 91 m 2 /g), whereas commercial ZnO-COM has a SSA of 5 m 2 /g. Meanwhile, this strategy via ZnCl 2 -KCl solid solution has also created a number of oxygen vacancies into ZnO aggregates. With these attractive features, as-made Pd-ZnO catalyst showed outstanding performance in methanol steam reforming, especially at low temperature (20 % Conversion and 95 % CO 2 Selectivity at 150 °C). Current strategy provides a gateway for the rational design of ZnO-based catalytic materials.
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高影响因子
CATALYSIS LETTERS
·
2021
·Vol. 152
·期 9
·2688-2694
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IF 3.186
Cai Mingzhong,Liu Rong,Xu Caifeng,Huang Bin
Pd(OAc) 2 /XPhos–SO 3 Na in a mixture of poly(ethylene glycol) (PEG-400) and water is shown to be a highly efficient catalyst for the cyanation of aryl chlorides with potassium ferrocyanide. The reaction proceeded smoothly at 100 or 120 ºC with K 2 CO 3 or KOAc as base, delivering a variety of aromatic nitriles in good to excellent yields. The isolation of the crude products is facilely performed by extraction with cyclohexane and more importantly, both expensive Pd(OAc) 2 and XPhos–SO 3 Na in PEG-400/H 2 O system could be easily recycled and reused at least six times without any apparent loss of catalytic efficiency. Graphical Abstract Palladium-catalyzed cyanation of aryl chlorides with potassium ferrocyanide leading to aryl nitriles by using Pd(OAc) 2 /XPhos–SO 3 Na/PEG-400/H 2 O as a highly efficient and recyclable catalytic system is described.
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高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2021
·
IF 19.503
Shufang Ji,Yuanjun Chen,Guofeng Zhao,Yu Wang,Wenming Sun,Zedong Zhang,Yong Lu,Dingsheng Wang
Atomic-level insight into the unique catalytic capability of single-atom catalysts that distinguished from nanometer-sized counterparts is highly desirable for catalyst design and catalysis research. By synthesizing single Pd atoms supported on TiO 2 as a catalyst, here we demonstrate a steric hindrance effect of single atoms induced by the unique isolation of single-atom active sites to achieve a remarkable enhancement on catalytic performance in the synthesis of dimethyl carbonate. Experimental results and density functional theory calculations reveal that such steric hindrance effect of single atoms favors the yield of the desired product dimethyl carbonate against further reacting with intermediates to form byproduct, because no extra Pd species around single Pd atoms provide active sites to further adsorb and activate substrates directly. The discovery of such steric hindrance effect is a valuable supplement to single-atom catalysis, and may promote single-atom catalysts to be widely applied in selective catalytic reactions .
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高影响因子
CHEMISTRY-A EUROPEAN JOURNAL
·
2021
·Vol. 27
·期 41
·10666-10676
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IF 5.236
Peng Zhang,Shaonan Xu,Yan Wang,Wei Zhang,Wenqing Li,Cundi Wei,Peiping Zhang,Shiding Miao
Graphical One man‘s trash is another man‘s treasure : A novel template strategy allows fibrous struvite—a composite Pd/Mg 2 P 2 O 7 with a mesoporous structure and an ultrahigh surface area—to be synthesized from wastewater. The prepared Pd/Mg 2 P 2 O 7 nanowires showed excellent performance in the selective hydrogenation of nitrobenzenes. This strategy provided a new pathway for synthesizing highly efficient catalysts as well as a solution for alleviate eutrophic pollution caused by N- and P-containing substances in wastewater. A highly efficient heterogeneous catalyst Pd/Mg 2 P 2 O 7 was fabricated by combining palladium nanoparticles (PdNPs) and mesoporous Mg 2 P 2 O 7 fibers/rods. Mg 2 P 2 O 7 fibers with ultra-high specific surface area were prepared from struvite as templates, which were synthesized from waste water containing N- and P-containing pollutants. This strategy provided a novel pathway for developing advanced catalysts from eutrophication-polluted water. The composite Pd/Mg 2 P 2 O 7 showed brilliant performance in selective hydrogenation of nitro aromatics to give anilines. As an example of nitrobenzene hydrogenation, the conversion to aniline and selectivity were found to reach almost 100 % at a temperature of T =90 °C and under a pressure of P =2.0 MPa. The superior performance was found to originate from PdNPs, which were boosted by electron transfer afforded by the nanofiber Mg 2 P 2 O 7 supports. The favorable adsorption of withdrawing groups (−NO 2 ) was realized by synergistic effects between Pd and oxygen vacancies provided by pyrolysis of struvite. The catalyst remained stable after cycles of reuse with little degradation in catalytic performance.
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高影响因子
CHINESE JOURNAL OF CATALYSIS
·
2021
·
IF 8.271
Dongyue Zhao,Yuexi Yang,Zhongnan Gao,Mengxin Yin,Ye Tian,Jing Zhang,Zheng Jiang,Xiaobo Yu,Xingang Li
Herein, we report the excellent De-NO x performance of La 0.7 Sr 0.3 MnO 3 (LSM) perovskite-supported Pd catalysts (Pd-LSM) in alternating lean-burn/fuel-rich atmospheres using C 3 H 6 as reductant and describe the in situ activation of the Pd catalysts via metal-support interaction (MSI) tuning. The NO x reduction conversion of the Pd-LSM catalyst increased significantly from 56.1% to 90.1% and the production of N 2 O was suppressed. Our results demonstrated that this behavior was mainly attributed to the in situ transformation of Pd 2+ into Pd 0 during the reaction. The generated Pd 0 species could readily activate the C 3 H 6 reductant and achieve an eight-fold higher turnover frequency than Pd 2+ for the reduction of NO x . Moreover, excessive MSIs inhibited the in situ generation of Pd 0 , and thereby, lowered the De-NO x activity of the catalyst even at high Pd dispersion. In addition, the Pd-LSM catalysts exhibited much higher S tolerance than conventional Al 2 O 3 -supported catalysts. Our study provides a new approach for analyzing and designing highly active metal catalysts operated under dynamic alternating oxidizing/reducing atmospheric conditions.
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高影响因子
APPLIED CATALYSIS A-GENERAL
·
2021
·
IF 5.706
Jiayu Song,Shengping Wang,Yan Xu,Qingling Liu,Yujun Zhao
Poor catalytic activity and stability are primary defects of traditional Pd/Al 2 O 3 catalysts for the low-temperature methane combustion. Herein, we developed a facile way to synthesize a MgAl-LDHs derived MgAl 2 O 4 spinel with good crystalline lattice and high surface area, which was used as support of Pd-based catalysts. Catalysts with Mg/Al ratio of 1/3 presented the highest methane combustion activity. It was found the well-crystallized MgAl 2 O 4 spinel promoted the dispersion and crystallization of PdO due to the strong interaction between PdO and support, and the electrophilicity and basicity originated from Mg doping suppressed the sintering of PdO particles, leading to the excellent performance of Pd/MgAl3. Moreover, these factors also inhibited the formation of surface OH- species, therefore, improved the water resistance. Such a synthesis strategy of the Pd/Mg x Al y derived from LDHs and the roles of MgAl 2 O 4 spinel could pose some meaningful directions for developing high-efficient Pd-based catalysts for the low-temperature methane combustion.
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