ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Cuizhen Yang,Tingyao Wang,Chengcheng Li,Haiyan He,Dongming Liu,Huajie Huang
In this study, we demonstrate a facile soft chemistry strategy for the in situ growth of two-dimensional (2D) ultrathin PdMo bimetallene tightly coupled with Ti3C2Tx MXene nanosheets (PdMo/Ti3C2Tx) using a robust stereoassembly process. The 2D PdMo bimetallene offers numerous unsaturated Pd atoms and simultaneously induces combined bimetallic alloy and strain effects, while the Ti3C2Tx matrix effectively optimizes the electronic structure of PdMo bimetallene via a face-to-face interface interaction and guarantees exceptional electrical conductivity. As a consequence, the newly designed PdMo/Ti3C2Tx nanoarchitecture expresses remarkable electrocatalytic properties for the formic acid and methanol electro-oxidation, in terms of large electrochemically active surface areas, ultrahigh catalytic activity, strong antipoisoning ability, and dependable long-term stability, all of which are better than those of conventional Pd nanoparticle catalysts supported by Ti3C2Tx and carbon matrices.
研究领域:
材料科学
·
电催化
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Materials Chemistry B
·
2021
·Vol. 9
·期 32
·6441-6459
·
IF 6.331
Lei Bai,Wenhui Yi,Yanru Wang,Yilong Tian,Baona Zhou,Tao Yi,Ping Zhang,Xin Cheng,Jinhai Si,Xun Hou,Jin Hou
By delivering the idea of green and safe hydrogen energy and novel photothermal therapy to the biomedical field, engineering of therapeutic nanomaterials for treatment of major diseases (such as cancer) holds great significance. In this work, a novel PdMo bimetallene was synthesized by a solvothermal reduction method, and it was explored and applied in the field of anti-tumor therapy for the first time. The absorption peak of the PdMo bimetallene can be precisely adjusted in the NIR biological window (700–1350 nm) only by changing the synthesis time. At the same time, it also shows strong light absorption and high photothermal conversion efficiency. Specifically, the photothermal conversion efficiencies at 808 nm, 980 nm and 1064 nm are 43.1%, 51.7% and 69.15%, respectively. Surprisingly, a PdMo bimetallene is an efficient catalyst, which can effectively promote hydrogen production from the hydrolysis of ammonia borane (AB) under acidic and photothermal conditions. Benefitting from these excellent properties, a multifunctional composite nano therapeutic agent (PdMo@AB@HA) was developed via layer-by-layer surface modification with AB and hyaluronic acid (HA). In this way, the synergistic PTT/hydrogen therapy of PdMo@AB@HA composite nanosheets in the NIR-I and NIR-II windows (808 nm, 980 nm, and 1064 nm) on mouse tumor xenografts of different depths was realized. Furthermore, the controlled release of hydrogen, targeted endocytosis, efficient eradication of tumors of different depths and high biosafety were systematically proved in vitro and in vivo. This work not only provides a novel and efficient theranostic nanoplatform for efficient cancer theranostics, but also provides a new strategy for the development of safe and efficient new anti-tumor therapies.
研究领域:
肿瘤学
·
纳米医学
·
生物材料学
·
光动力治疗
✓ 已验证
产品关联
DOI
PubMed
高影响因子
MICROCHIMICA ACTA
·
2021
·Vol. 188
·期 10
·1-11
·
IF 5.833
Yang Wei,Fan Lu,Guo Zhen,Wu Haiping,Chen Junman,Liu Changjin,Yan Yurong,Ding Shijia
A novel cytosensor was constructed for the ultrasensitive detection and nondestructive release of circulating tumor cells (CTCs) by combining Au nanoparticles-loaded two-dimensional bimetallic PdMo (2D Au@PdMo) nanozymes and electrochemical reductive desorption. The 2D Au@PdMo nanozymes possessed high-efficiency peroxidase-like activity and were assembled with an aptamer composed of a thiol-modified epithelial specific cell adhesion molecule (EpCAM) to strengthen CTCs adhesion. Moreover, the electrode surface was decorated with highly fractal Au nanostructures (HFAuNSs) composites due to the similarity in fractal nanostructure with the CTCs membrane to enhance the CTCs anchoring efficiency and release capability. The captured CTCs could be further efficiently dissociated and nondestructively released from the modified electrodes upon electrochemical reductive desorption. The designed cytosensor showed an excellent analytical performance, with a wide linear range from 2 to 1 × 10 5 cells mL −1 and low limit of detection (LOD) of 2 cells mL −1 (S/ N = 3) at the working potential in the range −0.6 to 0.2 V. A satisfactory CTCs release reaching a range of 93.7–97.4% with acceptable RSD from 3.55 to 6.41% and good cell viability was obtained. Thus, the developed cytosensor might provide a potential alternative to perform CTC-based liquid biopsies, with promising applications in early diagnosis of tumors. Graphical abstract
Preparation and mechanism of desorption of the cytosensor based on 2D Au@PdMo nanozymes and electrochemical reductive desorption for the detection and release of CTCs. A Preparation procedure of the Apt/Au@PbMo bioconjugates. B Fabrication process of the sandwich-type cytosensor. C Electrochemical signal produced by the Au@PdMo nanozymes. D Mechanism of electrochemical reductive desorption for CTCs release
研究领域:
生物医学工程
·
肿瘤学
·
纳米技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Advanced Energy Materials
·
2022
·Vol. 12
·期 26
·2200849
·
IF 29.698
Qianqian He,Tengfei Xu,Jiajie Li,Jialong Wang,Chunqiao Jin,Qian Chen,Xiaokang Gu,Xingguo Wang,Juntian Wei,Huiping Duan,Yongji Gong
One-dimensional (1D) ultrafine nanowires of different materials, especially noble metals, present an enticing prospect for catalyst applications due to their numerous active sites exposed. However, the controllable synthesis and stability issues hinder their practical applications. Herein, single-walled carbon nanotubes (SWCNTs) are adopted as the template to synthesize and stabilize ultrafine nanowires of metals. Furthermore, the oxygen reduction reaction (ORR) is employed as an application demonstration. Impressively, the as prepared PdMo nanowires exhibit a half-wave potential of 0.923 V and the mass activity is 35 times and 130 times higher than those of commercial Pt/C and Pd/C catalysts, respectively. Because of the protection, a superior ORR durability with 50 000 cycles can be achieved. Density functional theory (DFT) calculations reveal that the SWCNTs surface can be activated by the encapsulated PdMo NWs to achieve the exclusive adsorption of O 2 and the following reduction reaction. In addition, PdMo NWs@SWCNTs demonstrate excellent catalytic performance as the cathode of lithium-oxygen batteries. The cell can reach a high discharge capacity of over 10 000 mAh g −1 , better than most of the former reported catalytic electrodes. The tailored design PdMo NWs@SWCNTs show widespread applications in various energy storage & conversion fields.
研究领域:
纳米催化
·
能源材料
·
电化学
·
材料科学
·
计算化学
·
锂氧电池技术
✓ 已验证
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Huaifang Teng,Songliang Liu,Dalin Xu,Cong Zhang,Guangshuo Li,Meixiang Zheng,Xuejing Cui,Xin Chen,Luhua Jiang
Palladium (Pd) is one of the most promising catalysts for oxygen reduction reaction (ORR), however its activity is limited by the excessively strong adsorption of oxygen-containing intermediates. Herein, a one-dimensional (1D) ultrafine PdMo alloy nanowire (PdMo NWs) is synthesized, which exhibits excellent ORR activity and stability in both half cells and zinc-air batteries. The mass activity ( 1.08 mA μg Pd − 1 ) and specific activity (1.74 mA cm −2 ) of PdMo NWs are 9.2 and 6.9 times higher than that of a commercial nanosized Pt/C, respectively. Especially, the zinc-air battery with the PdMo NWs cathode achieves a peak power density of 214.8 mW cm −2 , and remains stable in a 160 h durability test. DFT calculations and in-situ electrochemical Fourier-transform infrared spectroscopy characterization reveal that the introduction of Mo significantly downshifts the d -band center of Pd, inhibiting excessive adsorption of the oxygen intermediates, thereby accelerating the ORR processes. This work demonstrates a 1D ultrafine Pd-based alloy nanowire as an effective and robust electrocatalyst for the ORR, and provides direct spectroscopic evidence for alleviated adsorption of oxygen intermediates on PdMo surfaces.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2024
·
IF 18.5
Wenxin Wang,Ruidong Yang,Qiqi Mao,Xu Mu,Hongjie Yu,Kai Deng,Jianguo Wang,Liang Wang,Hongjing Wang
The utilization of green hydrogen sources in H 2 O for alkynols electrocatalytic semihydrogenation reaction (ESHR) at ambient temperature provides a promising pathway toward the sustainable conversion of alkynols. However, it is still a great challenge to construct specific interfacial structure to adjust the electronic structure of Pd for the purpose of altering the strong adsorption of Pd with active hydrogen to enhance the production of alkenols. Here, the atomically dispersed GaO x -PdMo bimetallene nanoribbons (GaO x -PdMo BNRs) via oxygen bridging Ga atoms is designed to the surface of PdMo BNRs for 2-methyl-3-butyn-2-ol (MBY) ESHR to the synthesis of 2-methyl-3-buten-2-ol (MBE). The GaO x -PdMo BNRs achieve the excellent MBE selectivity (≈97.4%), Faraday efficiency (≈96.1%), and maintain long-term stability. Density functional theory demonstrates that the top electron-enriched Ga atoms and the bottom electron-deficient Pd atoms construct a “pyramidal” interface via the oxygen bridge. The unique surface can effectively activate H 2 O and weaken interaction between catalyst and MBE, thus promoting MBE generation. Moreover, the electron bridge effect between Ga-O-PdMo can induce p-d orbital hybridization to achieve lower the d -band center of surface Pd thus modulating the reactants adsorption. This work provides a strategy to improve ESHR performance by electron bridge effect to modulate interfacial electron distribution.
研究领域:
材料科学
·
催化化学
·
理论计算
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2024
·
IF 8.1
Cuizhen Yang,Tianyi Wang,Tingyao Wang,Haiyan He,Dongming Liu,Huajie Huang
The rapid development of direct formic acid fuel cell (DFAFC) and direct methanol fuel cell (DMFC) technologies urgently needs to explore efficient and multifunctional electrocatalysts with acceptable costs. In this work, we introduce a convenient soft-chemistry method for the bottom-up synthesis of two-dimensional (2D) ultrathin PdMo bimetallene in situ immobilized on reduced graphene oxide nanosheets (PdMo/RGO) by a robust stereoassembly procedure. The as-derived PdMo/RGO nanoarchitecture possesses a range of unique structural advantages tailored for anodic fuel cell systems , such as numerous exposed Pd atoms, bimetallic alloy and strain effects, stable 2D/2D heterointerfaces, and good electrical conductivity . As a result, the PdMo/RGO nanoarchitecture exhibits a large electrochemically active surface areas of 122.2 m 2 g −1 , a high mass activity of 994.8 mA mg −1 , as well as reliable long-term durability towards the formic acid oxidation reaction. Meanwhile, the PdMo/RGO electrocatalyst also displays exceptional electrocatalytic methanol oxidation performance with a mass activity of 1605.3 mA mg −1 in alkaline medium, which significantly surpasses that of conventional Pd nanoparticle catalysts loaded on reduced graphene oxide , carbon nanotube , and carbon black matrices.
✓ 已验证
产品关联
DOI
高影响因子
Catalysis Science & Technology
·
2026
·
IF 4
Ning He,Junqi Pei,Zixuan Zhang,Ruijun Hou
Acetylene hydrogenation provides a novel route to produce ethylene from coal or natural gas. However, the high concentration of acetylene would lead to considerable oligomerization. This work delves into the PdMo bimetallic system and addresses the critical challenge of catalyst deactivation in high-concentration acetylene hydrogenation. By using a rigorous method of external analysis with the incorporation of volume change before and after the reaction, the Pd/Mo composition dependence (Pd/Mo=3:1, 1:1 and 1:3) is examined, and a proper addition of Mo (Pd/Mo=1:1) can simultaneously maintain the hydrogenation activity as well as alkene selectivity, and significantly suppress the green oil selectivity compared with Pd/SiO2. The surface modification by Mo induces a Mo(δ⁺)-Pd(δ⁻) dual-site synergistic effect evidenced by density functional theory (DFT) calculations, and the elementary reaction pathways of hydrogenation and C2 dimerization are compared over the Pd(111) and Pd1Mo1(111) model surfaces. Consistently with experimental results, the bimetallic structure could effectively suppress the 1,3-butadiene (green oil precursor) formation. Therefore, the stability could be greatly enhanced over the PdMo bimetallic catalyst. This combined experimental and theoretical study reveals the underlying mechanism of the Mo modification in the inhibition of oligomerization, and provides guidance for efficient and stable catalyst design in the novel production of ethylene from a high-concentration acetylene feed.
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）