INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2018
·
IF 3.141
Yunpeng Zhou,Yangqiang Huang,Bo Jin,Xiao Luo,Zhiwu Liang
Pd nanoclusters supported on Schiff base modifying graphitic carbon nitride (Pd/u-CN100) had been successfully synthesized using urea and terephthalaldehyde as precursors by an impregnation approach. The resulting sheet materials exhibited high catalytic activity that turnover frequency rose to 98.9 h–1 and stability in CO2 hydrogenation. Various factors affecting formate production including the addition amount of TPAL, reaction pressure, reaction temperature, and catalyst stability testing were studied to achieve favorable catalytic conversion. An amount of characterization methods were applied to investigate the structure–activity relationship, including TEM, XRD, XPS, FTIR, HETEM, EDS, and BET. The high activity and stability might be resulted from the electronic modification, the relatively high dispersion of noble metal nanoclusters and the formation of intensely anchored metal-carrier bonds. More concretely, the scattered Schiff base loci and multiple nitrogen species were of great significance in the efficient and durable CO2 hydrogenation system.
研究领域:
材料科学
·
催化化学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
APL Materials
·
2023
·Vol. 11
·期 10
·
IF 6.1
Li Xia,Deng Min,Cao Tingting,Ma Jun,Geng Shuo,Ren Yuan,Yao Mengqin,Liu Fei,Dong Yonggang
Formic acid (FA, HCOOH), as a liquid chemical hydrogen storage carrier with low cost, high hydrogen content, and convenient storage and transportation, has attracted extensive attention. Pd-based catalysts for hydrogen production from FA are easy to aggregate and deactivate in the reaction process, which hinders the further development of FA as a hydrogen storage carrier. Therefore, the exploitation of carriers with simple preparation methods and excellent performance can effectively improve the catalytic activity of Pd-based catalysts. Porous carbon and SiO 2 have been widely used for their unique structural properties, and the preparation of composite carriers by combining the advantages of both is a current research hotspot. Herein, this work synthesized C–SiO 2 for the deposition of Pd nanoparticles by a one-step method, and the obtained Pd/C–SiO 2 exhibits a superior FA dehydrogenation activity with a turnover frequency value of 1278 h −1 and a favorable stability with only a slight decrease in activity after five cycles.
研究领域:
材料科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Nano Materials
·
2023
·
IF 5.9
Xiaoting Deng,Min Lao,Haikun Zhou,Jingwen Huang,Shihui Li,Yili Liang,Shaofeng Yin,Zhiyong Xie
The development of efficient catalysts for proton exchange membrane fuel cells (PEMFCs) is crucial for their commercial viability. This study introduces a method for synthesizing Pd nanoparticles on carbon supports as electrocatalysts using microbial synthesis, specifically employing the bacterium Shewanella oneidensis MR-1. The so-produced catalysts exhibit enhanced catalytic activity and stability for the oxygen reduction reaction (ORR). The microbial synthesis approach offers advantages, such as high purity, cost-effectiveness, and environmental friendliness. Additionally, the use of sodium alginate (SA) hydrogel in the synthesis process further improves the catalyst’s performance due to its metal chelating properties. The resulting Pd/C electrocatalysts, especially those synthesized with a composite matrix of SA and CaCO3, demonstrate superior ORR performances outperforming that of commercial Pd/C catalysts. It was found that the composite substrate affected the palladium recovery rate, whose increasing palladium absorption, refined particle size, improved graphitization degree, and increasing pyridinic-N of the resultant catalyst synergistically enhanced the availability of active centers that eventually contributed to the superior ORR performances. This research paves the way for the development of high-performance and cost-effective catalysts for PEMFCs.
研究领域:
材料科学
·
电化学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
NANOTECHNOLOGY
·
2022
·Vol. 33
·期 38
·385703
·
IF 3.953
Mei Zhang,Lin Cui,Qiqi Mao,Ziqiang Wang,Hongjie Yu,You Xu,Xiaonian Li,Liang Wang,Hongjing Wang
Exploring cost-effective and highly active electrocatalysts is of great significance for sustainable electrochemical NH3 synthesis. Palladium (Pd)-based catalysts have been unanimously considered as one of the most efficient catalysts for the nitrogen reduction reaction (NRR). Herein, self-supported mesoporous Pd film with partial oxidation on Ni foam (mPd-PdO/NF) was synthesized through the micelle-assisted chemical replacement method coupled with air oxidation under 260 °C, and the mPd-PdO/NF electrocatalyst exhibited superior NRR performance with the maximum values of rNH3 (24.8 mg h−1 mgcat.−1) and FE (16.64%) were obtained at −0.1 V, relative to the single counterparts (mPd/NF and mPdO/NF). It is proposed that both metallic Pd and its oxide domains when co-existing with a phase boundary between them can facilitate nitrogen activation and hydrogenation, resulting in an enhanced NRR performance. This work provides an inspiring strategy for the rational design of highly active and durable metal–metal–oxide nanoarchitectonics for ammonia electrosynthesis.
研究领域:
电化学
·
材料科学
·
催化
·
可持续化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Kai Guo,Hui Liu,Mengmeng Zhang,Nengyi Ni,Mengyao Mu,Ke Ren,Jiahui Chen,Qing Fan,Xueli Xu,Xiao Sun,Ximing Wang
Low-dose radiotherapy can lead to upregulation of PD-L1 expression in tumor cells, limiting the effectiveness of radio-immunotherapy. Currently, anti-PD-L1 drugs only disrupt the interaction of the PD-1/PD-L1 axis on the cell surface, without considering the immune regulatory ability of intracellular PD-L1. Additionally, antibody-bound PD-L1 can lead to internalization and recycling, allowing tumor cells to regain immune suppression. In this study, a novel PD-L1-affibody (Z PD-L1 )-grafted gadolinium-palladium nanoplatform incorporated with glucose oxidase (GOx) (GPGP) was fabricated to improve tumor-targeted magnetic resonance imaging (MRI) and synergistic radio-immunotherapy. GPGP with catalase- and peroxidase-like activity could catalyze the generation of oxygen to relieve tumor hypoxia and the generation of •OH to boost ferroptosis, respectively. GOx could enhance the nanoplatform’s dual nanozyme activity in a cascade, further sensitizing radiotherapy and intensifying subsequent immunogenic cell death. Crucially, GPGP induced AMPK phosphorylation and downregulated CMTM6, inhibiting intracellular PD-L1 production and blocking its transport to the cell membrane, thereby overcoming low-dose radiotherapy-induced PD-L1 upregulation. Systemic delivery of GPGP also demonstrated notable MRI contrast enhancement, providing precise imaging guidance for determining the optimal timing for radiotherapy. Therefore, GPGP has shown great potential in achieving effective MRI and collaborative tumor radio-immunotherapy.
研究领域:
肿瘤学
·
免疫学
·
纳米医学
·
放射生物学
✓ 已验证
产品关联
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2025
·
IF 7.3
Yan Shao,Jun Wan,Xiaoxia Ou,Cui Quan,Ningbo Gao,Xin Wang,Feng Zeng,Rongsheng Cai,Xiaolei Fan,Huanhao Chen
Engineering Pd–In2O3 interaction is key to developing catalysts with the desired CO2 hydrogenation activity toward methanol synthesis. Here, the crystalline phase of In2O3 nanospheres was tuned by changing the calcination temperature, which was found to affect the Pd–In2O3 interaction and thus the supported Pd states and CO2 hydrogenation performance of the prepared Pd/In2O3-a catalysts (where a refers to the calcination temperature for preparing In2O3). The fresh Pd/In2O3-a catalysts show varied initial activities, and after the induction period, their performance stabilized though being different. During the 100 h catalysis, catalyst microstructures changed, showing Pd aggregation and Pd–In alloying, which was related to the nature of the crystalline phase of In2O3. The hexagonal (h-In2O3) phase in Pd/In2O3-400 possesses concentrated surface OH groups and limited mobility. The relatively poor mobility limits Pd–In alloying, which possibly suppresses the hydrogen spillover effect, causing low CO2 conversion (8%) and methanol selectivity (45%) under steady-state conditions at 5 MPa and 300 °C. Conversely, the cubic In2O3 (c-In2O3) phase promotes Pd–In alloying and modifies Pd–In2O3 interaction during the reaction. The activity data show that Pd/In2O3-600 with the mixed phases of In2O3 (h/c-In2O3) demonstrated appropriate Pd–In2O3 interaction, leading to the Pd core InOx shell structure with the comparatively best methanol selectivity of about 65% at steady state. Conversely, Pd/In2O3-800 with the pure cubic In2O3 (c-In2O3) phase and a relatively low specific surface area of 16 m2 g–1 encourages the sintering of Pd and thereby the formation of homogeneous Pd–In alloys, having a moderate methanol selectivity of about 50%. These findings highlight the importance of the In2O3 crystal phase engineering in the catalytic CO2 hydrogenation over Pd/In2O3 catalysts and the dynamics of Pd–In interactions, which affect the methanol yield.
研究领域:
催化化学
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材料科学
·
能源化学
✓ 已验证
产品关联
DOI
高影响因子
NANOTECHNOLOGY
·
2022
·Vol. 33
·期 21
·210001
·
IF 3.953
Yiwen Chen,Junguo He,Peigen Jiang,Heliang Pang,Xuhui Hu,Jie Zhang,Wenjing Zhang
The growing chloramphenicol (CAP) in wastewater brought a serious threat to the activity of activated sludge and the spread of antibiotics resistance bacteria. In this study, a highly ordered nanoporous Co3O4 layer on Co foil through anodization was prepared as cathode for nitro-group reduction and electrodeposited with Pd particles for dechlorination to reduce CAP completely. After 3 h treatment, almost 100% of CAP was reduced. Co2+ ions in Co3O4 served as catalytic sites for electrons transfer to CAP through a redox circle Co2+–Co3+–Co2+, which triggered nitro-group reduction at first. With the presence of Pd particles, more atomic H* were generated for dechlorination, which increased 22% of reduction efficiency after 3 h treatment. Therefore, a better capacity was achieved by Pd/Co3O4 cathode (K = 0.0245 min−1, K is reaction constant) than by other cathodes such as Fe/Co3O4 (K = 0.0182 min−1), Cu/Co3O4 (K = 0.0164 min−1), and pure Co3O4 (K = 0.0106 min−1). From the proposed reaction pathway, the ultimate product was carbonyl-reduced AM (dechlorinated aromatic amine product of CAP) without antibacterial activity, which demonstrated this cathodic technology was a feasible way for wastewater pre-treatment.
研究领域:
环境科学
·
化学工程
·
生物医学工程
✓ 已验证
DOI
PubMed
高影响因子
BIOMATERIALS
·
2025
·
IF 12.9
Zhanxue Xu,Xinrui Yang,Xingyu Lu,Dandan Su,Yidan Wang,Huixing Wu,Zhenhua Zhang,Changrui Long,Liqian Su,Yanyu Wang,Hongbo Chen,Shijian Xiang,Benjie Zhou
Combination therapies for melanoma face challenges due to asynchronous drug delivery and associated toxicity, underscoring the need for advanced delivery systems. While immune checkpoint inhibitors (ICIs) enhance T cell activity, optimal cytotoxic responses require efficient antigen presentation by mature dendritic cells (DCs), which are often functionally impaired in the tumor microenvironment. Thus, effective treatment requires coordinated T cell activation, DC-mediated priming, and direct tumor suppression. Herein, wild Glycyrrhiza uralensis Fisch roots-derived nanovesicles (GC NV) are demonstrated to be effective inhibitors of melanoma proliferation. The vesicles exert this activity through the intracellular delivery of encapsulated miRNA (miR2916) and bioactive molecules (isoliquiritigenin), with this capacity for intracellular delivery extending to the STING agonist DMXAA. We also demonstrate how chemical modification can be used to install PD-L1 antibodies on the membrane surface of these GC NV, imbuing these vesicles with selectivity for tumor cells. Combining DMXAA encapsulation with surface-displayed PD-L1 antibodies creates vesicles (GP@DMX NV) that both promote DCs maturation and elicit CD8 + T cell response. Our multifunctional GP@DMX NV reverse the immunosuppressive microenvironment of melanoma and significantly enhance the immunotherapeutic potential of immune checkpoints.
研究领域:
肿瘤学
·
药剂学
·
免疫学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ENERGY & FUELS
·
2019
·
IF 3.021
Bingxing Jiang,Jun Hu,Yiheng Qiao,Xiaoxiang Jiang,Ping Lu
Performance of Ni–Pd bimetallic catalysts on depolymerization of lignin into monomeric phenols was investigated using isoproponal as an in situ hydrogen source. The performance of catalysts and the effects of temperature and starting lignins were extensively examined. Ni50Pd50/SBA-15 exhibited the best performance in the depolymerization of cellulolytic enzyme corn stalk lignin, affording the highest total monophenols yield of 8.14 wt % which was 1.96 times that of Ni/SBA-15 and 1.44 times that of Pd/SBA-15. For the depolymerization of acid-extracted birch lignin, 18.52 wt % monophenols were obtained over Ni50Pd50/SBA-15 at 245 °C for 8 h, and 4-propylsyringol had 8.89 wt % yield with 47.97% selectivity. The physicochemical characteristics of the catalysts were elucidated with ascanning electron microscopy, high-resolution transmission electron microscopy, nitrogen adsorption/desorption, X-ray diffraction, and X-ray photoelectron spectroscopy. The bimetallic catalyst had the characteristics of narrow distribution of metal particles with a small size, well-retained hexagonal pore structure of SBA-15, higher dispersion of Pd, and more Pd0 and Ni0 as compared with monometallic catalysts. The properties of the bimetallic catalyst provide more contact opportunities between the abundant active centers and lignin fragments, and therefore significantly promote the hydrogenolysis process to produce monomeric phenols.
研究领域:
化学工程
·
催化科学
✓ 已验证
产品关联
DOI
高影响因子
Molecular Catalysis
·
2023
·
IF 4.6
Haoquan Guo,Xinyu Lu,Yue Yang,Jinhe Wei,Lizhi Wu,Li Tan,Yu Tang,Xiaoli Gu
Alkyl phenol is an essential chemical intermediate that is in high demand in the chemical industry. The synthesis of alkyl phenols from lignin-derived molecules is one of the most promising routes for utilizing biomass resources. Herein, we report the catalytic hydrodeoxygenation (HDO) of dihydroeugenol (DHE) to alkyl phenols over a highly dispersed Pd/α-MoC catalyst with a substrate conversion of 98% and a selectivity of 96% to alkyl phenols. The Pd/α-MoC catalyst prepared by co-precipitation and temperature-programmed carbonization exhibits exceptional HDO activity under mild conditions with a low H 2 pressure (1–10 bars). The characterizations of the catalyst suggest that Pd are highly dispersed on the α-MoC matrix. The reaction mechanism was investigated using the substrate scope experiments. Under ambient pressure, the abundant oxygen vacancies and acidity sites on Pd/α-MoC enable the selective hydrodeoxygenation of lignin monomers.
研究领域:
化学工程
·
生物质利用
✓ 已验证
产品关联
DOI
高影响因子
Molecular Catalysis
·
2024
·
IF 3.9
Chi Ma,Zhiyong Zhong,Quanjun Xiang
The photocatalytic efficiency of bismuth-based metal-organic framework (Bi-MOF) is extremely restricted by the rapid recombination of photogenerated electron-hole pairs, which reduce the number of electrons involved in the photocatalytic reduction reaction. Constructing precise interfacial bond bridges between metal nanoparticles (NPs) and MOFs has emerged as an effective strategy to address the above-mentioned issues, promoting the electrons transfer. Herein, this study improves the sluggish dynamics of photogenerated charge in Bi-MOF by inducing the Pd-O-Bi bond bridges at the interface on a Pd NPs-decorated Bi-MOF (Pd/Bi-MOF) nanosheets. This phenomenon results in an interaction between Pd NPs and the Bi-MOF support. And Pd-O-Bi bond bridges provide the fast electron transfer channels, triggering the directional migration of photogenerated electrons from Pd to Bi node, then enhancing the spatial separation of photogenerated electron-hole pairs, finally facilitating overall photocatalytic CO 2 reduction. The presence of these bond bridges leads to higher enhancement in CO production for Pd/Bi-MOF nanosheets compared to the Bi-MOF nanosheets under visible light irradiation after 4.5 h. This research demonstrates the importance of interfacial bond bridges and provides a reasonable guide to design efficient photocatalyst for reduction of CO 2 to CO.
研究领域:
材料科学
·
环境科学
·
化学
✓ 已验证
产品关联
DOI
高影响因子
Frontiers of Chemical Science and Engineering
·
2024
·Vol. 18
·期 11
·1-11
·
IF 4.3
Gao Huimin,Zhang Jinpeng,Zhang Fangyuan,Jing Jieying,Li Wen-Ying
The photocatalytic reduction of CO 2 into formic acid is a feasible approach to alleviate the effects of global climate change and achieve chemical energy storage. It is important to design highly active photocatalysts to improve the selectivity and yield of formic acid. In this study, TiO 2 -based catalysts were prepared and loaded with Pd nanoparticles via an impregnation process. The Pd/H-TiO 2 catalyst demonstrated superior CO 2 reduction activity and a high formic acid production rate of 14.14 mmol cat ·g −1 ·h −1 . The excellent catalytic performance observed in the presence of a Pd/H-TiO 2 catalyst is ascribed to the synergy between O v and Pd. The presence of O v led to increase in CO 2 adsorption while Pd loading enhanced the photogenerated electron-hole pair separation. Electron transfer from H-TiO 2 to Pd also contributed to CO 2 activation.
研究领域:
环境科学
·
材料科学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）