CHEMICAL ENGINEERING JOURNAL
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2023
·
IF 15.1
Entong Ye,Zheng Chen,Yongyong Shi,Dan Zhang,Wenfei Li,Hong Qin,Ziming Luo,Quansheng Wu,Qian Lin,Hongyan Pan,Keliang Wang
Although a high-activity yield of hydrogen peroxide (H 2 O 2 ) can be achieved by direct synthesis from hydrogen and oxygen, developing an extreme catalyst with high activity and stability is still very challenging, which limits its industrial application. Here, we reported a catalyst Pd/SPE with polyelectrolyte membranes SPE as an electronic acceptor to anchor Pd, which achieves H 2 O 2 selectivity of 90.1% and productivity of 5764.4 mmol∙g Pd -1 ∙h −1 . The results of TEM, XRD and ICP-MS, XPS, CO-DRIFT, O 2 -TPD, synchrotron radiation and density functional theory (DFT) simulations reveal that the electrons of Pd are transferred into polyelectrolyte membranes and Pd clusters are strongly chemisorbed on SPE, which is beneficial for O 2 adsorption and inhibits the dissociation of O-O bond, leading to significantly enhanced H 2 O 2 productivity and selectivity.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2023
·
IF 8.6
Lili Zhang,Hailong Lu,Jinxia Ma,Yimin Fan,Zhiguo Wang,Yonghao Ni
The separation and reusability of nano-catalysts are paramount for their high-efficiency and low-cost use. Herein, lignocellulose hydrogels (LCG), were fabricated and served as the host matrix for in-situ generated palladium nanoparticles (Pd NPs), creating hydrogel-based Pd NPs reactor systems. The lignocellulose hydrogel-based Pd NPs (LCG/Pd NPs) reactor system possesses the following unique features: (1) lignin present in LCG acts as a “green” reducing agent so that Pd NPs are formed in situ; (2) the in-situ generated Pd NPs are well dispersed in the LCG structure via complexation; (3) the simultaneous adsorption-catalysis process concept is very effective for pollutant remedy: the adsorption of pollutants on the porous LCG effectively increases the pollutant concentration on the reaction sites, where the Pd NPs are co-located, enhancing the catalytic reactions; as a result, a much higher catalytic reaction rate is observed; (4) the LCG/Pd NPs reactor systems are readily reused/recycled after each use. As proof of this concept, the catalytic performance of the LCG/Pd NPs reactor system was demonstrated by the catalytic reduction of toxic heavy metal ions (Cr 6+ ) and organic dye (methyl orange). Results showed that the novel LCG/Pd NPs reactor system exhibited much increased catalytic reduction rates: the pseudo-first-order rate constant (k) is 118 times higher (from 0.018 to 2.129 min −1 at 25 °C) for MO, and 38 times higher (from 0.008 to 0.304 min −1 at 25 °C) for Cr 6+ , in comparison with the control, under otherwise the same conditions.
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Foods
·
2023
·Vol. 12
·期 17
·3319
·
IF 5.2
Zainabu Majid,Qi Zhang,Zhansen Yang,Huilian Che,Nan Cheng
In modern agricultural practices, organophosphorus pesticides or insecticides (OPs) are regularly used to restrain pests. Their limits are closely monitored since their residual hinders the capability of acetylcholinesterase (AChE) and brings out a threatening accumulation of the neurotransmitter acetylcholine (ACh), which affects human well-being. Therefore, spotting OPs in food and the environment is compulsory to prevent human health. Several techniques are available to identify OPs but encounter shortcomings like time-consuming, operating costs, and slow results achievement, which calls for further solutions. Herein, we present a rapid colorimetric sensor for quantifying OPs in foods using TMB as a substrate, a multi-enzyme cascade system, and the synergistic property of core-shell Palladinum@Platinum (Pd@Pt) nanoparticles. The multi-enzyme cascade response framework is a straightforward and effective strategy for OPs recognition and can resolve the previously mentioned concerns. Numerous OPs, including Carbofuran, Malathion, Parathion, Phoxim, Rojor, and Phosmet, were successfully quantified at different concentrations. The cascade method established using Pd@Pt had a simple and easy operation, a lower detection limit range of (1–2.5 ng/mL), and a short detection time of about 50 min. With an R2value of over 0.93, OPs showed a linear range of 10–200 ng/mL, portraying its achievement in quantifying pesticide residue. Lastly, the approach was utilized in food samples and recovered more than 80% of the residual OPs.Keywords:Pd@Pt nanoparticles;organophosphorus pesticides;acetylcholinesterase;colorimetric detection;multi-enzyme cascade
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Catalysts
·
2023
·Vol. 14
·期 1
·24
·
IF 3.9
Chunlian Luo,Luwei Chen,Abdullah N. Alodhayb,Jianhua Wu,Mingwu Tan,Yanling Yang
The development of catalysts for low-temperature methane combustion is crucial in addressing the greenhouse effect. An effective industrial catalyst strategy involves optimizing noble metal utilization and boosting metal–metal interaction. Here, the PdNi-H catalyst was synthesized using the self-assembly method, achieving the high dispersion and close proximity of Pd and Ni atoms compared to the counterparts prepared by the impregnation method, as confirmed by EDS mapping. The XRD and TEM results revealed Pd2+and Ni2+doping within the CeO2lattice, causing distortions and forming Pd-O-Ce or Ni-O-Ce structures. These structures promoted oxygen vacancy formation in CeO2, and this was further confirmed by the Raman and XPS results. Consequently, the PdNi-H catalyst demonstrated an excellent redox ability and catalytic activity, achieving lower ignition and complete methane burning temperatures at 282 and 387 °C, respectively. The highly dispersed PdNi species played a pivotal role in activating methane for enhanced redox ability. Additionally, the narrow size distribution range contributed to more vacancies on the surface of CeO2, as confirmed by the XPS results, thereby facilitating the activation of gas phase oxygen to form oxygen species (O2−). This collaborative catalytic approach presents a promising strategy for developing efficient and stable methane combustion catalysts at low temperatures.
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Small
·
2020
·Vol. 16
·期 52
·2004879
·
IF 11.459
Liang Zhao,Yingli Luo,Qiaoyi Huang,Ziyang Cao,Xianzhu Yang
Blocking immune checkpoint pathways with an antibody or small interfering RNA (siRNA) has become a promising method to reactivate antitumor responses for cancer treatment. However, both blockade strategies achieve only temporary inhibition of these immune checkpoints. Herein, a photoswitched CRISPR/Cas9 system for genomic disruption of the PD-L1 gene is developed to achieve permanent blockade of the PD-1/PD-L1 pathway; this system is constructed by using a photoactivated self-degradable polyethyleneimine derivative and the plasmid pX330/sgPD-L1 (expression of the Cas9 protein and single-guide RNA targeting PD-L1). Under light irradiation, this photoswitched CRISPR/Cas9 system efficiently genetically disrupts the PD-L1 gene in not only bulk cancer cells but also cancer stem-like cells. As a result, the photoswitched CRISPR/Cas9 system significantly increases the infiltration of CD8 + T cells into tumor tissue, leading to effective activation of a T cell-mediated antitumor response against cancer cells and cancer stem-like cells. This study provides an alternative strategy to block the PD-1/PD-L1 pathway for efficacious immune checkpoint therapy.
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Journal of Materials Chemistry A
·
2020
·Vol. 8
·期 37
·19300-19308
·
IF 11.301
Jingchun Wang,Xiaoyu Qiu,Keying Su,Siyuan Wang,Jiatian Li,Yawen Tang
It remains a grand challenge to control the island growth mode because a conformal growth is theoretically more favorable, in which the lattice mismatch between the overlayer and the substrate is negligible. Herein, we report the first example of “Frank–van der Merwe” mode and “Volmer–Weber” mode of Pd atoms on Boerdijk–Coxeter-type helical Au(111) nanowires. Quantitative analyses suggest that the pH-induced faster kinetic reduction rate (1.2 × 10−2 s−1) is a crucial factor to switch the Pd-growth mode from the conformal 4-atom-layers to ultrasmall islands. As a proof-of-concept application, the VW Au@Pd HNWs exhibit outstanding ORR activity (Eonset = 1.07 V, E1/2 = 0.91 V) and stability, outperforming FM Au@Pd NWs, Au(111) NWs, Pd black, and most reported electrocatalysts. Physical characterization systematically elucidated similar components, d-band center locations, and lattice distortions of both the representative structures, giving brand-new insights into the impact of their slightly different surface microstructures. In particular, the segmented oxyphilic–anaerobic interface of the VW Au@Pd HNWs directly balances the adsorbability of the intermediates; meanwhile, the interleaved lattice orientations favor multi-directional electron transmissions to promote ORR kinetics. This finding not only challenges the conventional wisdom of lattice-matched growth but also provides an identical model for the in-depth understanding of the structure–function relationship with a focus on the growth modes.
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CHEMICAL ENGINEERING JOURNAL
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2020
·
IF 10.652
Mingxin Lv,Yanwei Zhang,Qianghua Xin,Defu Yin,Shitao Yu,Shiwei Liu,Lu Li,Congxia Xie,Qiong Wu,Hailong Yu,Yue Liu
In this work, a series of Pd@Al-MSiO 2 yolk–shell-structured nanospheres (YSNSs) with different Al contents were synthesized by a facile one-pot method. The EDX elemental analysis and high-magnification TEM image of Pd@Al-MSiO 2 YSNSs confirmed that its well-defined yolk-shell structure with a moving Pd core and mesoporous silica shell rich in Al species. Furthermore, Solid state NMR and Py-FTIR results confirmed that Al species grafting mainly formed 4-coordinated Al (AlO 4 ) in the mesoporous silica framework which led to generating abundant Lewis acid sites. The influence of Al species on the physicochemical properties of Pd@Al-MSiO 2 YSNSs, as well as their catalytic performance for the hydrogenolysis of glucose to 1,2-propylene glycol (1,2-PG), was investigated. The mesoporous silica shell with abundant Lewis acid sites is a significant contributor to the isomerization of glucose into fructose, while the Pd core plays a role in promoting the hydrogenation of intermediates. The unique hollow space inside the Pd@Al-MSiO 2 YSNSs provides a location for the retro -aldol condensation of fructose and consequently avoids direct hydrogenation of fructose. The as-synthesized Pd@Al 3 -MSiO 2 YSNSs shows superior catalytic activity (1,2-PG selectivity of 47.4%, glucose conversion of 95.4%) in the hydrogenolysis of glucose, and far outperforms the Pd/Al 3 -MSiO 2 catalysts. In addition, owing to the influence of the 4-coordinated Al species on the geometry and chemical properties of the mesoporous silica shell, the nanospheres show good stability and reusability over multiple catalytic cycles without significant loss of activity.
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Theranostics
·
2020
·
IF 8.579
Yu Zhang,Quanyi Liu,Chong-Bo Ma,Qingqing Wang,Meiting Yang,Yan Du
Alcohol abuse causes health problems and security accidents. A reliable and sensitive detection system for alcohol has been an instinctive demand in law enforcement and forensic. More efforts are demanded in developing new sensing strategy preferably with portable and non-invasive traits for the pushforward of point-of-care (POC) device popularization. Methods : We developed a POC diagnosis system for alcohol assay with the aid of alcohol oxidase (AOX) pre-joining in the system as well as Pd@Pt core-shell nanoparticles (abbreviated to Pd@Pt) that were decorated on ploy(vinyl alcohol) aerogel with amphiphilicity. Biological samples like saliva and whole blood can be absorbed by the aerogel in a quick process, in which the analyte would go through a transformation from alcohol, H 2 O 2 , to a final production of O 2 , causing an analyte dose-dependent signal change in the commercial portable pressure meter. The cascade reactions are readily catalyzed by AOX and Pd@Pt, of which the latter one possesses excellent peroxidase-like activity. Results : Our design has smartness embodied in the aerogel circumvents the interference from methanol which is more ready to be catalyzed by AOX. Under the optimal conditions, the limit of detection for alcohol was 0.50 mM in saliva, and is able to distinguish the driving under the influence (DUI) (1.74 mM in saliva) and driving while impaired (DWI) (6.95 mM in saliva) in the national standard of China. Conclusion : Our proof-of-concept study provides the possibility for the establishment of POC device for alcohol and other target detection, not only owing to the sensing qualification but also thanks to the architecture of such sensor that has great flexibility by replacing the AOX with glucose oxidase (GOX), thenceforth realizing the accurate detection of glucose in 0.5% whole blood sample. With the advantages of easy accessibility and anti-interference ability, our sensor exhibits great potential for quantitative diagnostics in biological system.
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Molecular Catalysis
·
2021
·
IF 5.062
Guoliang Gao,Huangze Yu,Xue Lu Wang,Ye-Feng Yao
The alloy catalyst formed by transition metal and a small amount of noble metal has become the most promising substitute for M-based ( M = Pt, Pd, Ru, Rh) catalyst. However, due to the direct exposure of the metal core to the electrolyte, it is vulnerable to corrosion and oxidation, which in turn reduces the catalytic stability and is becoming a major obstacle to sustainable hydrogen production. The present work addresses this issue by developing a one-step immersion-adsorption-pyrolysis strategy for synthesizing FeM alloy nanoparticles with N-doped carbon coatings (FeM@CN) for use as electrocatalysts in the HER. The deliberately designed metal-organic framework material was used as the precursor of catalyst synthesis to achieve the carbon coatings and simultaneously the heteroatom in-situ doping for the alloy nanoparticles. The optimal FePt@CN demonstrates excellent catalytic stability and HER activity in an acidic electrolyte medium. The reactions obtain a small overpotential of 28 mV to achieve current densities of 10 mA cm −2 , which are comparable to a high-performance commercial Pt/C electrocatalyst with a much higher Pt loading. The FeRu@CN also demonstrates an outstanding performance with an overpotential of only 18 mV to achieve a current density of 10 mA cm −2 in an alkaline medium.
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JOURNAL OF NANOBIOTECHNOLOGY
·
2021
·Vol. 19
·期 1
·1-23
·
IF 10.435
Jiang Weixi,Su Lei,Ao Meng,Guo Xun,Cheng Chen,Luo Yuanli,Xie Zhuoyan,Wang Xingyue,Wang Junrui,Liu Shuling,Cao Yang,Li Pan,Wang Zhigang,Ran Haitao,Zhou Zhiyi,Ren Jianli
Background Recent studies have demonstrated that multidrug resistance (MDR) is a critical factor in the low efficacy of cancer chemotherapy. The main mechanism of MDR arises from the overexpression of P-glycoprotein (P-gp), which actively enhances drug efflux and limits the effectiveness of chemotherapeutic agents. Results In this study, we fabricated a “combo” nanoagent equipping with triple synergistic strategies for enhancing antitumor efficacy against MDR cells. Tumor homing-penetrating peptide endows the nanosystem with targeting and penetrating capabilities in the first stage of tumor internalization. The abundant amine groups of polyethylenimine (PEI)-modified nanoparticles then trigger a proton sponge effect to promote endo/lysosomal escape, which enhances the intracellular accumulation and retention of anticancer drugs. Furthermore, copper tetrakis(4-carboxyphenyl)porphyrin (CuTCPP) encapsulated in the nanosystem, effectively scavenges endogenous glutathione (GSH) to reduce the detoxification mediated by GSH and sensitize the cancer cells to drugs, while simultaneously serving as a photoacoustic imaging (PAI) contrast agent for image visualization. Moreover, we also verify that these versatile nanoparticles in combination with PD-1/PD-L1 blockade therapy can not only activate immunological responses but also inhibit P-gp expression to obliterate primary and metastatic tumors. Conclusion This work shows a significant enhancement in therapeutic efficacy against MDR cells and syngeneic tumors by using multiple MDR reversing strategies compared to an equivalent dose of free paclitaxel. Graphic Abstract
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Molecular Catalysis
·
2021
·
IF 5.062
Pan Tian,Zhongjie Cai,Guowu Zhan,Jiale Huang,Qingbiao Li
The conversion of CO 2 into value-added chemicals is an effective way to mitigate the environmental problems caused by huge anthropogenic CO 2 emissions. Although In 2 O 3 /Pd catalyst possesses excellent catalytic performance in CO 2 hydrogenation to methanol, the formation of Pd-In alloy on the catalyst surface greatly reduces the yield of methanol. Herein, we adopt a natural biomaterial ( viz. , rape pollen) as a template to synthesize hierarchically structured bio-In 2 O 3 and bio-In 2 O 3 /Pd catalysts. In particular, we found that the pretreatment of pollen using hydrochloric acid (HCl) played a critical role in determining catalytic performance. A series of bio-In 2 O 3 were prepared by using the pollen templates with different etching degrees, and then the bio-In 2 O 3 -x/Pd catalysts (x denoted as the amount of HCl, mL) were prepared using an impregnation-reduction method. It was surprising that the CO 2 conversion of bio-In 2 O 3 –15/Pd catalyst was 8.2% with methanol selectivity of 74.7%, which was much better than the bio-In 2 O 3 –0/Pd (2.6% and 54.6%, respectively). The dramatic enhancement was due to that the acid-etched pollen template owns a hollow cage-like structure and abundant surface functional groups (-NH 2 and -COOH), which is beneficial to the growth of In 2 O 3 with a high amount of surface oxygen vacancies. Also, the bio-In 2 O 3 /Pd catalyst (prepared with untreated pollen template) was more prone to form Pd-In alloys as a result of the strong interaction between Pd with In 2 O 3 . In contrast, the In 2 O 3 spatial distribution of bio-In 2 O 3 –15/Pd was more uniform with an appropriate interaction of Pd with In 2 O 3 that inhibited the formation of Pd-In alloys. Even Pd loaded on commercial In 2 O 3 exhibited inferior performance (3.4% CO 2 conversion and 81% methanol selectivity) to bio-In 2 O 3 –15/Pd catalyst. Accordingly, the present work offers a green and efficient method to prepare supported In 2 O 3 /Pd catalysts by using the acid-etched pollen as a template.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2021
·
IF 5.816
Na Ye,Zhao Jiang,Tao Fang
The low-palladium Pd/TaN–C catalyst is synthesized by a surfactant-free solvothermal approach and exhibits high activity (2613.18 mA mg Pd −1 ), durability and CO tolerance for MOR (methanol oxidation reaction) in alkaline media , 12.4 folds that of the commercial Pd/C. XPS and electrochemical results indicate that the interfacial Pd–TaNO bond is generated. This also brings the enhancement of OH ad adsorption responsible for anti-CO poisoning ability. Density Functional Theory (DFT) calculations indicate that the reaction pathway and the rate-determining step are changed for methanol decomposition to CO on the Pd 4 /TaN(001) surface compared with Pd (111). The preferred pathway can be described as: CH 3 OH→CH 3 O→CH 2 O→CHO→CO. Furthermore, the results indicate that the adsorption of OH is enhanced and the energy barrier of COOH formation from CO + OH is reduced with the high concentration of hydroxyl on the Pd 4 /TaN(001) surface, further confirming the bi-functional effect of hydroxyl on the CO tolerance.
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