Chemical Engineering Journal Advances
·
2021
·
IF 0
Haidong Liu,Jingrui Shang,Lingjian Zeng,Binbin Cao,Hongbo Geng,Jianping Lang,Xueqin Cao,Hongwei Gu
Developing stable, efficient and economical electrocatalytic materials is still challenging for hydrogen evolution reaction (HER). Hence, we develop a Pd/Ni bimetallic carbon electrocatalyst (Pd/Ni-NC) with outstanding electrocatalytic performance. The catalyst derived from Pd-doped Ni-MOF (Pd/Ni-MOF) has particles and needle-like carbon tubes on its surface and is similar in shape to setaria. Benefiting from the composition and the unique structure, Pd/Ni-NC shows excellent HER catalytic performance with 16 mV at 10 mA cm −2 , superior to Pd or Ni single metal-carbon catalyst. Furthermore, it maintains stable catalytic activity under constant current for 25h. These results show the strategy that obtaining Pd and Ni bimetallic MOF by cation exchange and its corresponding bimetallic carbon material with setaria-shaped structure by calcination is powerful for high efficient HER performance.
研究领域:
材料科学
·
电化学
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DOI
Journal of Materials Chemistry B
·
2022
·Vol. 10
·期 8
·1291-1300
·
IF 7.571
Simeng Wei,Xinxin Shao,Yong Liu,Boyu Xiong,Pengfei Cui,Ziling Liu,Quanshun Li
Immune checkpoint blockade therapy against programmed death protein-1 and its ligand (PD-1/PD-L1) has been accepted as a promising approach to activate the immune system's anti-tumor response. Although small interfering RNA (siRNA) or antibodies can block the PD-1/PD-L1 pathway, the effect of this blockade is temporary and reversible. Here, we developed a nano-delivery system to achieve permanent disruption of the PD-L1 gene based on Clustered Regularly Interspaced Short Palindromic Repeats (CRISPR)/CRISPR-associated nuclease 9 (Cas9) gene editing technology. In this system, the CRISPR/Cas9 plasmid was delivered into melanoma B16F10 cells using a nucleobase-modified polyamidoamine (PAMAM) derivative namely AP-PAMAM, which was constructed through the modification with 2-amino-6-chloropurine. Meanwhile, the carrier could efficiently facilitate the endosomal escape of CRISPR/Cas9 plasmid and thereby inhibit PD-L1 expression in cancer cells. Moreover, the intravenous injection of AP-PAMAM/plasmid nanoparticles could recruit and activate CD8+ T cells at the tumor site, promoting the secretion of cytokines and the killing of tumor cells. Overall, this nano-delivery system for genome editing provided a promising strategy to block the PD-1/PD-L1 pathway and obtain effective tumor immunotherapy.
研究领域:
癌症免疫学
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基因治疗
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纳米技术
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分子生物学
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DOI
PubMed
高影响因子
APPLIED SURFACE SCIENCE
·
2026
·
IF 6.6
Le Yu,Hong Li,Zhaoyi Xu,Shourong Zheng,Tao Long,Wang Lei
Ultrafine Pd nanoparticles were stabilized on aminopropyl-functionalized SBA-15. • The catalyst enabled efficient FA decomposition and TCE hydrochlorination. • Successful TCE removal was achieved through FA-driven catalytic hydrogenation. Trichloroethylene (TCE), a persistent and highly toxic groundwater contaminant, demands efficient remediation strategies. Formic acid (FA, HCOOH)-assisted catalytic hydrodechlorination (HDC) is a promising approach for TCE removal, with Pd-based catalysts exhibiting excellent activity for both FA dehydrogenation and C-Cl bond hydrogenation. This study investigates an amino-functionalized SBA-15-supported Pd catalyst (Pd/SBA-15-NH 2 ) for TCE degradation in the FA-driven hydrogenation system. TEM and XPS characterization showed that the amino groups significantly enhance Pd dispersion and stabilize positively charged Pd δ+ species, furthermore in-situ DRIFTs tests conclusively confirmed that HCOO* species serve as the key intermediates in the FA dehydrogenation process, DFT study also showed Pd/SBA-15-NH 2 have lower free energy and thus improve the activity of FA dehydrogenation. Kinetic analysis confirmed a pseudo-first-order pathway with an TOF of 208.6 h −1 and apparent activation energy of 46.6 kJ/mol. Under optimized conditions (pH = 5.6, 25 °C), the catalyst achieved 100% TCE conversion in 120 min with a initial activity of 0.072 mM/(g min). Meanwhile, ethane (C 2 H 6 ) as the dominant reaction product, indicating that TCE degradation proceeds via a one-step rather than dechlorination mechanism. These findings provide valuable insights for catalytic dichlorination mechanism for chlorinated ethenes, while highlighting the theoretical foundation for the development of high-performance, noble metal-based catalysts in environmental applications. Download: Download high-res image (107KB) Download: Download full-size image
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DOI
高影响因子
JOURNAL OF CATALYSIS
·
2026
·
IF 6
Hao Niu,Jiaqi Song,Lixia Yang,Liangjiu Bai,Kun Yin,Donglei Wei,Hou Chen,Huawei Yang
Solar-driven hydrogen peroxide (H 2 O 2 ) synthesis from water and oxygen stands as a sustainable and viable strategy, yet its progress remains constrained by the lack of high-performance photocatalysts. Here we report a Pd atomic site on tetrakis (4-carboxyphenyl) porphyrin supramolecular nanosheet catalyst for photocatalytic H 2 O 2 production. The optimized catalyst achieves an exceptional H 2 O 2 yield rate of 608 μmol g −1 h −1 under visible light. A combination of experimental investigations and theoretical simulations verifies that the H 2 O 2 generation proceeds via a dual-pathway mechanism, encompassing both the oxygen reduction reaction (ORR) and the water oxidation reaction (WOR). The Pd atomic sites not only enhance visible-light absorption and facilitate charge transport, but also serve as efficient electron traps that significantly lower the energy barriers for the formation of key intermediates (*OOH for the ORR pathway and *OH for the WOR pathway). This work presents a high-performance photocatalytic system and delivers atomic-scale insights into the sustainable solar-driven H 2 O 2 synthesis process.
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Zhiqiang Zhao,Yiwen Huang,Minghao Chao,Silin Du,Junjie Li,Jin Wang,Guangyu Ma,Yufan Liu,Xin Kang,Mengying Fu,Dehong Yu,Shibao Li,Fenglei Gao
Oxygen defect engineering, which precisely modulates the coordination environments and dynamic equilibria of oxygen vacancies (O v ), lattice oxygen (O lat ), and adsorbed oxygen (O ads ), serves as a pivotal strategy for optimizing electronic structures and catalytic pathways in metal oxides and is expected to become a core means to enhance the activity of nanoenzymes. Leveraging optimized component ratios from oxygen defect engineering, we engineered hollow porous nanocages with a distinctive 3D open framework to maximize active site exposure. Controlled reduction reconstructed oxygen species distribution, endowing the material with exceptional peroxidase (POD), oxidase (OXD), and laccase (LAC) activities. Capitalizing on phenolic pollutants' structural features and reducibility, we developed a tri-channel nanozyme sensor array using CuO@Pd nanocages. This system enables efficient oxidative degradation and precise identification of six phenolic compounds through synergistic triple-enzyme catalysis. Transcending the pH limitations of conventional sensors, the array differentiates phenolic analogues across concentrations with broad linear ranges and high sensitivity. This work establishes a direct methodology for modulating nanozyme activity via oxygen defect engineering while elucidating the electron-transfer mechanism in Pd Cu redox cycling.
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产品关联
DOI
高影响因子
Reaction Chemistry & Engineering
·
2025
·
IF 3.1
Hongbo Yu,Weixing Ming,Wei Wei,Yanan Zhao,Xin Dong,Xianguo Wu,Gaowu Qin,Dongmao Yan
Amines represent crucial intermediates in fine chemical synthesis, finding extensive applications across pesticide, dye, and pharmaceutical industries. N,N-Dimethyl tertiary amines can be efficiently synthesized through reductive amination of dimethylamine. We developed an environmentally benign continuous flow reductive amination system employing a micro-packed bed reactor (μ-PBR) with a Pd/C catalyst prepared via direct impregnation. This system successfully produces N,N-dimethylcyclohexylamine (DMCHA) in an aqueous system, achieving high selectivity (99.5%), impressive space–time yields (2.7 × 104 g L−1 h−1), and operates without requiring additional additives. In addition, the reaction system demonstrated excellent stability during a 120-hour continuous test and proved suitable for both aromatic aldehydes and aromatic amines.
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产品关联
DOI
高影响因子
JOURNAL OF CATALYSIS
·
2025
·
IF 6.5
Juhong Nie,Xuelian Li,Yixin Zhang,Jinghui Zheng,Yajun Qiu,Han Yan,Wensheng Yan,Yu Xiong,Jia Guan,Jian Zhang
Hydrodeoxygenation is the key technology for realizing the conversion of biomass into high value-added chemicals, but usually encounters low efficiency and harsh conditions due to the rich electron density and strong C-O bonds of O-containing groups. Herein, an efficient catalyst is precisely constructed with abundant acidic O dopants and well-exposed oxidized Pd centers for hydrodeoxygenation of vanillin. Through a tannic acid-assisted strategy, it is precisely constructed on alumina that electron-deficient O species doped as ether types in carbon along with ultra-small PdO nanoparticles. The collaboration of acidic sites from O dopants and oxidized Pd centers on PdO boosts hydrodeoxygenation of vanillin into valuable 2-methoxy-4-methylphenol in 99 % yield with a turnover frequency value of 752 h −1 under mild conditions (80 °C, 0.5 MPa H 2 ), significantly surpassing similar catalysts without oxidized Pd centers or O dopants as well as commercial Pd heterogeneous and homogeneous catalysts. Further theoretical calculations disclose that oxidized Pd centers are superior to metallic Pd centers for hydrogenating vanillin aldehyde group, which is revealed to stabilize the reaction system and facilitate the adsorption of H 2 , while the acidic O dopants play a crucial role in promoting the subsequent alcohol-based deoxygenation process by facilitating the C-O bond cleavage synergistically.
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产品关联
DOI
高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2023
·
IF 9.5
Yan Chen,Shao-Chun Wu,Jiao-Jiao Han,Xi Yan,Xiao-Jing Guo,Wan-Zhong Lang
Catalytic Pd decorated graphene oxide (Pd/GO) membrane with efficient catalytic activity was developed by in-situ reduction of Pd 2+ on GO nanosheets followed by vacuum filtration. A high 4-nitrophenol (4-NP) reduction efficiency was achieved by using the Pd/GO catalytic membrane with layered structure because of evenly distribution of Pd nanoparticles (NPs) in the interlayer space of GO membrane, ensuring sufficient contact between 4-NP molecules and Pd NPs. The apparent kinetic rate constant and turnover frequency (TOF) reached to 138.4 s −1 and 813 h −1 under a continuous-flow system using 4000 mg/L of 4-NP at 20 °C. During a 300 min of continuous-flow catalysis, the 4-NP conversion was kept above 98% at 20 °C. This high catalytic efficiency of the Pd/GO catalytic membrane under high 4-NP concentration and continuous-flow catalysis made it promising and competitive in the application of catalytic membrane for efficient catalytic process.
研究领域:
材料科学
·
环境科学
·
催化化学
✓ 已验证
DOI
高影响因子
JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY
·
2026
·
IF 1.6
Mao Yiyin,Zhou Peng,Jiang Juntao,Liu Yaling,Wang Hongyong,Han Guoqing,Wu Jun,Zou Pei,Lu Chunxiong
Programmed death-ligand 1 (PD-L1) represents a pivotal target for immune checkpoint blockade therapy. This study developed a novel PD-L1-targeting SPECT probe [ 99m Tc]Tc-G 3 C-2CBM based on dimeric 2-bromo-3-biphenyl (CBM) scaffold design. The probe was designed to enable bivalent interactions through dual CBM domains, exhibiting > 98% radiochemical yield and excellent in vitro stability. Cellular uptake studies revealed significantly higher accumulation in PD-L1-overexpressing A375-hPD-L1 cells compared to A375 cells (14.15 ± 2.11% vs. 5.89 ± 0.55% at 4 h; uptake ratio = 3.20). The probe displayed favorable binding affinity (K D = 36.54 ± 7.28 nM) and inhibitory potency (IC 50 = 69.62 ± 5.15 nM). In vivo SPECT imaging confirmed tumor-specific accumulation, though accompanied by notable hepatic uptake. These results demonstrate that CBM dimerization is a feasible approach for retaining PD-L1 binding and may provide a basis for the future development of multivalent radiotracers.
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DOI
高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
·
2024
·
IF 8
Xuan-Yu Yang,Hao-Nan Chen,Li-Juan Yue,Fei-Long Gong,Ke-Feng Xie,Shi-Zhong Wei,Yong-Hui Zhang
The design of novel functional nanostructures for advanced chemical engineering field is of great importance. In this work, Pd-modified Na-doped WO 3 nanorods are rationally designed for rapid and detection of hydrogen, which is a green and clean energy in modern industry. Notably, and H + as well as citrate ions play an important role in the formation of 1D nanorods, and the morphology formation mechanism is explored. Here, inspired by the novel Pd-modified Na-doped WO 3 nanorods structure, the Pd-400-Na/WO 3 NRs exhibit high sensing ability with ultra-high response to hydrogen (R a /R g = 218@25 ppm) and fast response time (3 s). The combination of experimental and theoretical results shows that Na doping effectively modulates the d-band center of Pd and enhances activation and desorption of H 2 on the Pd surface. The 1D porous structure also facilitates the diffusion of H 2 within the framework, and accelerate the charge transformation. Meanwhile, the surface Pd 0 sites are assigned as the surface active sites for H 2 adsorption and activation, and Pd 2+ sites facilitate the desorption process. Our work paves the new insights for the design of high performance H 2 sensing materials.
研究领域:
材料科学
·
化学工程
·
纳米技术
✓ 已验证
DOI
高影响因子
WATER RESEARCH
·
2017
·
IF 6.942
Yuancai Lv,Zhuyu Niu,Yuancai Chen,Yongyou Hu
With the introduction of nano zero valent iron (nZVI) technology into our environment, its potential environmental risk to environmental microorganisms has attracted considerable attention. In this study, Pseudomonas putida was chosen as a typical strain to study the bacterial toxicity of nZVI/Pd. The CFU assay results indicated that nZVI/Pd was toxic to P. putida cells but the toxicity decreased with an increase in DO. The experiments isolated by dialysis bag and flow cytometry analysis suggested that both membrane disruption caused by direct contact and oxidative stress were the main bactericidal mechanisms under the aerobic condition , while membrane disruption resulting from direct contact was the primary bactericidal mechanism in the anaerobic system. Furthermore, according to TEM, SEM, EDS , XRD , FTIR and XPS , it was indicated that in the aerobic system, the reactive oxygen species (ROS) generated by nZVI/Pd could oxidize the amide and hydroxyl groups into carboxyl groups , resulting in a decline in peptides and increase in polysaccharides . In addition, the ROS also accumulated inside the cell and caused cell inactivation via oxidative stress . In the anaerobic system, the adhered nZVI/Pd particles would attack the functional groups such as carboxyl, ester and amide, leading to the decline in proteins and polysaccharides and subsequent damage of the membrane. The findings provide a significant guide for the application of nano-bio combined technology.
研究领域:
环境微生物学
·
纳米生物学
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DOI
高影响因子
Nature Communications
·
2024
·Vol. 15
·期 1
·1-10
·
IF 14.7
Wang Hengjia,Qin Ying,Wu Yu,Qiu Yiwei,Ling Ling,Fang Qie,Wang Canglong,Hu Liuyong,Gu Wenling,Zhu Chengzhou
Hydrogen adsorption and desorption in single-phase catalysts often occur at a single catalytic site based on the traditional hydrogen evolution reaction (HER) pathway, which makes it difficult to break the limitation entailed by the Sabatier principle. Herein, β-Pd hydride metallene (β-PdHene) aerogels are synthesized as advanced HER catalysts. A lattice hydrogen-involved mechanism is reported to separate adsorption and desorption sites, which is thermodynamically favorable compared to the traditional reaction pathway. In situ differential electrochemical mass spectrometry and theoretical calculations reveal that lattice hydrogen as additional active sites directly participate in the HER process. Consequently, β-PdHene aerogels exhibit a low overpotential of only 20 mV at 10 mA cm −2 and remarkable HER stability, which are even comparable to commercial Pt/C. Our work opens an avenue to rationally develop highly active HER catalysts, bypassing the design limitations of catalysts under traditional mechanisms.
研究领域:
材料科学
·
化学工程
·
催化
·
电化学
✓ 已验证
DOI
高影响因子
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