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APPLIED CATALYSIS B-ENVIRONMENTAL · 2023 · IF 22.1

Electrocatalytic upcycling of polyethylene terephthalate plastic to formic acid coupled with energy-saving hydrogen production over hierarchical Pd-doped NiTe nanoarrays

Hugang Zhang,Yile Wang,Xinmiao Li,Kai Deng,Hongjie Yu,You Xu,Hongjing Wang,Ziqiang Wang,Liang Wang

Electrochemical upcycling of plastic waste to high-value chemicals is an ideal approach for the valorization of waste resources. In this study, we report the electro-reforming of polyethylene terephthalate (PET) plastic hydrolysate to valuable formate and hydrogen. Pd-deposited hierarchical aligned NiTe nanoarrays on Ni foam (Pd-NiTe/NF) is developed for oxidation of PET hydrolysate at anode and hydrogen evolution at cathode, with the overpotentials of 0.019 and 1.35 V at 10 and 100 mA cm -2 , respectively. In co-electrolysis system, the Pd-NiTe/NF exhibits high Faradaic efficiencies for concurrent production of value-added formate (95.6%) and H 2 (98.6%). The high activity and stability of Pd-NiTe/NF can be ascribed to that the interfacial heterostructures by incorporating Pd atoms and the strongly interfacial electronic interactions of between Pd and NiTe can synergistically promote PET-derived ethylene glycol to formate oxidation and hydrogen evolution. This work shows promising prospect in electro-reforming PET plastic waste to valuable chemicals.

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Bioactive Materials · 2022 · IF 16.874

A tumor cell membrane-coated self-amplified nanosystem as a nanovaccine to boost the therapeutic effect of anti-PD-L1 antibody

Zhilin Li,Hao Cai,Zhiqian Li,Long Ren,Xuelei Ma,Hongyan Zhu,Qiyong Gong,Hu Zhang,Zhongwei Gu,Kui Luo

To improve the response rate of immune checkpoint inhibitors such as anti-PD-L1 antibody in immunosuppressive cancers like triple-negative breast cancer (TNBC), induction of immunogenic cell death (ICD) at tumor sites can increase the antigenicity and adjuvanticity to activate the immune microenvironment so that tumors become sensitive to the intervention of immune checkpoint inhibitors. Herein, a self-amplified biomimetic nanosystem, mEHGZ, was constructed by encapsulation of epirubicin (EPI), glucose oxidase (Gox) and hemin in ZIF-8 nanoparticles and coating of the nanoparticles with calreticulin (CRT) over-expressed tumor cell membrane. EPI acts as an ICD inducer, Gox and hemin medicate the cascade generation of reactive oxygen species (ROS) to strengthen the ICD effect, and CRT-rich membrane as “eat me” signal promote presentation of the released antigens by dendritic cells (DCs) to invoke the tumor-immunity cycle. The biomimetic delivery system displays an amplified ICD effect via Gox oxidation, hydroxyl radical generation and glutathione (GSH) depletion. The induced potent ICD effect promotes DCs maturation and cytotoxic T lymphocytes (CTLs) infiltration, reversing an immunosuppressive tumor microenvironment to an immunoresponsive one. Treatment with the nanosystem in combination with anti-PD-L1 antibody results in distinctive inhibition of tumor growth and lung metastasis, supporting that a potent ICD effect can significantly boost the therapeutic efficacy of the anti-PD-L1 antibody. This self-amplified biomimetic nanoplatform offers a promising means of raising the response rate of immune checkpoint inhibitors.

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BMC Medicine · 2022 ·Vol. 20 ·期 1 ·1-18 · IF 11.15

Combination of an autophagy inhibitor with immunoadjuvants and an anti-PD-L1 antibody in multifunctional nanoparticles for enhanced breast cancer immunotherapy

Cheng Yibin,Wang Caixia,Wang Huihui,Zhang Zhiwei,Yang Xiaopeng,Dong Yanming,Ma Lixin,Luo Jingwen

Background The application of combination therapy for cancer treatment is limited due to poor tumor-specific drug delivery and the abscopal effect. Methods Here, PD-L1- and CD44-responsive multifunctional nanoparticles were developed using a polymer complex of polyethyleneimine and oleic acid (PEI-OA) and loaded with two chemotherapeutic drugs (paclitaxel and chloroquine), an antigen (ovalbumin), an immunopotentiator (CpG), and an immune checkpoint inhibitor (anti-PD-L1 antibody). Results PEI-OA greatly improved the drug loading capacity and encapsulation efficiency of the nanoplatform, while the anti-PD-L1 antibody significantly increased its cellular uptake compared to other treatment formulations. Pharmacodynamic experiments confirmed that the anti-PD-L1 antibody can strongly inhibit primary breast cancer and increase levels of CD4+ and CD8+ T cell at the tumor site. In addition, chloroquine reversed the “immune-cold” environment and improved the anti-tumor effect of both chemotherapeutics and immune checkpoint inhibitors, while it induced strong immune memory and prevented lung metastasis. Conclusions Our strategy serves as a promising approach to the rational design of nanodelivery systems for simultaneous active targeting, autophagy inhibition, and chemotherapy that can be combined with immune-checkpoint inhibitors for enhanced breast cancer treatment.

CAS / MDL: 9002-98-6 112-80-1
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International Journal of Nanomedicine · 2022 · IF 7.033

Multifunctional Nanoparticles-Mediated PTT/PDT Synergistic Immune Activation and Antitumor Activity Combined with Anti-PD-L1 Immunotherapy for Breast Cancer Treatment

Cunqing Kong,Banghao Xu,Guanhua Qiu,Meng Wei,Mengqi Zhang,Shengxian Bao,Jiali Tang,Lequn Li,JunJie Liu

Introduction Photoimmunotherapy is a breakthrough treatment for malignant tumors. Its uniqueness is that it uses antibody mediated targeted delivery to achieve high tumor specificity and uses laser-activated biophysical mechanism to accurately induce the rapid death of cancer cells and avoid damaging the surrounding normal tissues. Methods In this paper, an iron-based micelle was designed to encapsulate the photothermal agent indocyanine green (ICG) and a cyclic tripeptide of arginine-glycine-aspartic acid (cRGD) as targeted multifunctional ICG@SANPs-cRGD nanoparticles for combined photothermal/photodynamic/immune therapy of breast cancer. Results The experimental results show that ICG@SANPs-cRGD nanoparticles have good biocompatibility and photothermal conversion ability. Photothermal therapy (PTT) and photodynamic therapy (PDT) based on ICG@SANPs-cRGD can not only inhibit the proliferation, invasion and migration of tumor cells, but also directly kill tumor cells by inducing apoptosis or necrosis. Dual-mode fluorescence light (FL) and magnetic resonance imaging (MRI) imaging in mice confirmed the selective accumulation at tumor sites and imaging ability of ICG@SANPs-cRGD. PTT/PDT combined with Anti-PD-L1 immunotherapy based on ICG@SANPs-cRGD mediated the immunogenic cell death (ICD) of tumor cells by regulating the expression of immune-related indicators and activated the body's immune response mechanism, which enhanced the immunotherapy effect of immune checkpoint block (ICB). PTT/PDT combined with Anti-PD-L1 therapy not only prevented the progression of the primary tumor but also inhibited the distant metastasis of the tumor. Discussion This study explores the biomedical application of PTT/PDT combined with Anti-PD-L1 based on ICG@SANPs-cRGD nanomaterials for breast cancer treatment and demonstrates the potential of ICG@SANPs-cRGD as a multifunctional therapeutic platform for future cancer therapy.

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Nanoscale Advances · 2022 ·Vol. 4 ·期 19 ·4162-4168 · IF 5.598

A fine single Pd microwire H2 sensor fabricated by using a femtosecond laser for a wide detection range at room temperature

He Zhu,Yun-Zhi Dai,Xiang-Chao Sun,Hong Xia

We reported a fine H2 sensor based on single Pd microwires (SPMs) by femtosecond-laser-induced deposition of palladium nanoparticles (PdNPs), which exhibits excellent H2 sensing performance. The PdNPs with good dispersion were prepared by ultrasonic assisted one-step solution synthesis. The sensor has a wide detection range of 0.001–4.0% H2 sensing at room temperature. With the increase of the H2 concentration, the SPM sensor presents two sensing mechanisms, the formation of PdHx and hydrogen induced lattice expansion regulating the conductivity of SPMs. This fine hydrogen sensor is promising to be applied to human health monitoring, environmental air detection and other integrated intelligent devices.

CAS / MDL: 16940-66-2
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INORGANIC CHEMISTRY · 2022 · IF 5.436

One Stone Two Birds: Unlocking the Synergy between Amorphous Ni(OH)2 and Pd Nanocrystals toward Ethanol and Formic Acid Oxidation

Hu Yang,Aichuang Zhang,Yunfei Bai,Mingyu Chu,Han Li,Yuan Liu,Peng Zhu,Xiaolei Chen,Chengwei Deng,Xiaolei Yuan

Even though extensive efforts have been devoted to mixing Pd nanocrystals with Ni(OH)2 for the enhanced synergy, it remains a great challenge to incorporate nanosized Ni(OH)2 species on the Pd electrode and reveal their synergy. Herein, we present spongelike Pd nanocrystals with the modification of amorphous Ni(OH)2 species. The catalyst configuration is first considered by compositing Pd with Ni(OH)2 species to optimize the Pd–Pd interatomic distance and then constructing a strongly coupled interface between Pd nanostructures and Ni(OH)2 species. For the ethanol oxidation reaction (EOR) and the formic acid oxidation reaction (FAOR), Pd-Ni(OH)2 composites exhibit an impressive mass activity of 4.98 and 2.65 A mgPd–1, respectively. Most impressively, there is no significant decrease in the EOR activity during five consecutive cycles (50 000 s). A series of CO-poisoning tests have proved that the enhanced EOR and FAOR performances involve synergy between Pd nanostructures and Ni(OH)2 species.

CAS / MDL: 7585-39-9 10025-98-6
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JOURNAL OF MOLECULAR LIQUIDS · 2022 · IF 6.633

A separation strategy of Au(III), Pd(II) and Pt(IV) based on hydrophobic deep eutectic solvent from hydrochloric acid media

Ronghao Liu,Jinjie Hao,Yangyang Wang,Yuanyuan Meng,Yanzhao Yang

A hydrophobic deep eutectic solvent (HDES) based on lidocaine and thymol was examined for selective extraction and separation of Au(III), Pd(II) and Pt(IV) in the acidic leaching solution of secondary resources. At first, the properties of HDES were characterized by 1 H NMR, DSC, TGA, RDF and ESP to prove its suitability for extraction process. In addition, extraction behaviors, maximum extraction capacities and competitive extraction experiment were investigated to explore the extraction ability of HDES. The results show that the maximum extraction capacity of Au(III), Pd(II) and Pt(IV) reached 761.2 g/L, 98.3 g/L and 299.3 g/L, respectively. Meanwhile, their extraction efficiency was affected by the changing acidity of aqueous. And then, ion-association mechanism in the extraction process was proposed through the analysis of FT-IR. Finally, a separation process was proposed for the recovery of Au(III), Pd(II) and Pt(IV) based on acidity control and KSCN, which achieved recovery efficiency of 97.8 % Au(III), 99.9 % Pd(II) and 89.5 % Pt(IV). After collecting and regenerating the used HDES, their extraction performance of Au(III), Pd(II) and Pt(IV) were still maintained.

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SEPARATION AND PURIFICATION TECHNOLOGY · 2022 · IF 9.136

Toward green and efficient recycling of Au(III), Pd(II) and Pt(IV) from acidic medium using UCST-type ionic liquid

Yangyang Wang,Shuwen Chen,Ronghao Liu,Lixin Zhang,Wenfeng Xue,Yanzhao Yang

The development of efficient ionic liquids (ILs) for disposable separation and recovery of various precious metals was of great importance, but still faced difficult challenges. A phase change temperature-controlled system composed of IL and HCl solution was developed for the extraction and separation of Au(III), Pd(II) and Pt(IV) from secondary resources. UCST (upper critical solution temperature)-type IL ([1,4,7-TMTA][Tf 2 N]) possessed outstanding selectivity of precious metals and the property of temperature-controlled phase transition. The ability of ILs to form solvated hydrogen bonds was confirmed by quantum-chemical calculation to be correlated with their corresponding UCST. Different experimental parameters were optimized to explore the extraction behavior of IL. It is noteworthy that homogeneous liquid-liquid extraction system (HLLE) constructed by UCST-type IL could significantly enhance the extraction kinetic of Au(III), Pd(II) and Pt(IV) by decreasing phase interface resistance. For Au(III), Pd(II) and Pt(IV), when the system temperatures were higher than 40 °C, 49 °C and 65 °C, the maximum values were 98.5%, 98.3% and 93.2% at the highest efficiency. In addition, the extraction mechanism of anion exchange was revealed by UV–vis, IR, NMR and LC-MS spectrometry. At last, Au(III), Pd(II) and Pt(IV) could be selectively separated from multi-metal solutions where impurity ions coexist by K 2 C 2 O 4 , NH 3 ·H 2 O and CS(NH 2 ) 2 /HCl, respectively. After 5 cycles, the extraction performance of [1,4,7-TMTA][Tf 2 N] maintained. In summary, this paper overcame the obstacle of slow kinetics of solvent extraction technology, and pointed out a way for polymetallic co-extraction and separation in HLLE system.

CAS / MDL: 90076-65-6 105-39-5
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Reaction Chemistry & Engineering · 2022 ·Vol. 7 ·期 8 ·1827-1835 · IF 5.2

Liquid-phase catalytic hydrodechlorination of chlorinated organic compounds in a continuous flow micro-packed bed reactor over a Pd/AC catalyst

Zipin Peng,Xuepeng Wang,Zheng Li,Xingkun Chen,Yunjie Ding,Jisong Zhang

Catalytic hydrodechlorination (HDC) is considered to be a safe and effective method to treat chlorinated organic pollutants and has always been a hot spot in basic catalysis research. It is difficult to obtain excellent catalytic performance due to the inferior mass transfer performances of traditional batch reactors, and the deactivation of catalysts can easily occur due to the poisoning effect of HCl. In this work, Pd catalysts supported on activated carbon (Pd/AC) were synthesized by the ion-exchange (IE) method. The characterization results of N2 physisorption, XRD, TEM and XPS revealed that the active Pd components were uniformly dispersed on the surface of AC in the form of nanoparticles. A continuous flow system based on a micro-packed bed reactor (μPBR) was developed for the hydrodechlorination, and the hydrogenation of chlorobenzene (CB) was selected as the model reaction. With the optimal reaction conditions, a conversion and selectivity of 100% were obtained. Importantly, no obvious deactivation of the catalysts was observed during a 100 h time-on-stream test. Moreover, Pd/AC catalysts exhibited remarkable substrate suitability in dechlorination systems. The reaction kinetics for hydrodechlorination of CB in methanol was investigated after the internal and external diffusion limitations were eliminated.

CAS / MDL: 67-56-1
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APPLIED CATALYSIS B-ENVIRONMENTAL · 2022 · IF 24.319

Ultralow-content Pd in-situ incorporation mediated hierarchical defects in corner-etched Cu2O octahedra for enhanced electrocatalytic nitrate reduction to ammonia

You Xu,Kaili Ren,Tianlun Ren,Mingzhen Wang,Ziqiang Wang,Xiaonian Li,Liang Wang,Hongjing Wang

Electrochemical reduction of nitrate (NO 3 - ) to ammonia (NH 3 ) offers a sustainable avenue to close the NO 3 - cycle for NH 3 synthesis. Critical to the feasibility of electrochemical NO 3 - -to-NH 3 technology is the development of cost-effective, scalable and selective catalysts that can produce NH 3 with high yield. To this end, we design and constructure ultralow-content Pd (2.93 at%) in-situ incorporated Cu 2 O corner-etched octahedra (Pd-Cu 2 O CEO) with cavity and oxygen vacancy defects for selectively electrochemical NO 3 - -to-NH 3 transformation. The unique conner-etched cavity structure, rich surface oxygen vacancies, and Pd-Cu 2 O dual active sites, synergistically promote nitrate electroreduction undergo ammonia formation reaction pathway. Impressively, the as-made Pd-Cu 2 O CEO exhibited outstanding activity for electrocatalytic NO 3 - -to-NH 3 , with high ammonia selectivity (95.31%) and Faradaic efficiency (96.56%). The developed hierarchical-defect strategy may open a new avenue for reasonable design of defect electrocatalysts to contribute desirable properties and functionalities in specific applications.

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SEPARATION AND PURIFICATION TECHNOLOGY · 2023 · IF 8.6

Pd nanoparticles supported on microflower NiMOF modified roughed nickel foam with the enhanced active site for electrochemical dechlorination of trichloroacetic acid

Fangyuan Wang,Yuanyuan Li,Huanqing Xie,Chunyu Wu,Wen Gao,Jianping Qiu,Lexing You,Shuang Song

Electrocatalytic hydrodechlorination (ECH) has been considered as an effective method to convert refractory chlorinated organics into biodegradable chlorine-free organics under mild conditions. In this work, a composite electrode of Pd/NiMOF/roughed nickel foam (Pd/NiMOF/RNF) with excellent dechlorination performance was prepared by electrodeposition of Pd nanoparticles on the flower-shaped NiMOF interlayer grown in-situ . Benefiting from the high specific surface area of NiMOF structure and excellent dispersion of Pd facilitated, the Pd/NiMOF/RNF offered abundant active hydrogen and larger open channels for the easy diffusion of reactants and products in the electrochemical dechlorination process. 97% of 6 μmol/L trichloroacetic acid (TCAA) was dechlorinated at a cathodic potential of −1.2 V within 90 min. The corresponding palladium mass activity was calculated to be 0.39 μg min −1 cm −2 mg −1 Pd, which was approximately 3.5 times greater than other report on ECH cathode. Moreover, the Pd/NiMOF/RNF cathode remained stable even after five consecutive cycle tests. Toxic assessment results indicated that the dechlorination process was beneficial to the detoxification of TCAA at the end of reaction. The hydrodechlorination mechanism of TCAA was proposed by density functional theory (DFT) analysis and electrochemical characterization on the Pd/NiMOF/RNF electrode. The findings of this study have the potential to contribute to the development of electrocatalytic treatment methods for chlorinated organic compounds in drinking water.

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Acta Pharmaceutica Sinica B · 2021 · IF 11.614

The cellular immunotherapy of integrated photothermal anti-oxidation Pd–Se nanoparticles in inhibition of the macrophage inflammatory response in rheumatoid arthritis

Chuping Zheng,Aiping Wu,Xinyun Zhai,Hong Ji,Zhikang Chen,Xu Chen,Xiyong Yu

Reducing the inflammatory response is a major goal in the therapy of rheumatoid arthritis (RA). Herein, we integrated palladium nanoparticles (Pd NPs) with selenium nanoparticles (Se NPs) and obtained a multiple nanosystem ( [email protected] NPs) that could simultaneously scavenge hydroxyl radicals (⋅OH) and provide a photothermal effect. The [email protected] NPs were constructed by a simple self-assembly method in which Se NPs were electrostatically bonded to Pd NPs; hyaluronic acid (HA) was linked to the NPs by ester bonding to provide macrophage targeting ability. The experiments show that the combined therapy of eliminating ⋅OH with Se NPs and utilizing PTT with Pd NPs could effectively reduce the inflammatory response in macrophages more effectively than either individual NP treatment. In addition, the outer layer of HA could specifically target the CD44 receptor to enhance the accumulation of [email protected] NPs at the lesion, further enhancing the therapeutic effect. After treatment for 15 days, the [email protected] NPs nearly eliminated the inflammatory response in the joints of mice in an induced RA model, and prevented joint damage and degradation.

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