JOURNAL OF CATALYSIS
·
2020
·
IF 7.888
Zhe Han,Chizhou Tang,Jijie Wang,Landong Li,Can Li
Hydrogenation of CO 2 into methanol using the H 2 produced from renewable energy is a promising way for carbon capture and utilization. Therefore, the methanol synthesis catalysts with high methanol selectivity are highly desired. In this work, we found that the methanol selectivity of In 2 O 3 catalyst can be significantly enhanced by introducing a small amount of Pt. Methanol selectivity can be increased from 72.2% (In 2 O 3 ) to 91.1% (0.58 wt.% Pt/In 2 O 3 ) at 220 °C. The introduced Pt atoms are doped into the In 2 O 3 , forming atomically dispersed Pt n+ species, most of which are stable under working conditions. It is proposed that the atomically dispersed Pt n+ species are responsible for the enhanced methanol selectivity, while Pt nanoparticles on In 2 O 3 mainly boost the reverse water-gas shift reaction (CO 2 + H 2 → CO + H 2 O).
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Junlin Cai,Xinyan Liao,Pingting Li,Qiuxiang Wang,Hongpu Huang,Zixi Lyu,Jing Lin,Shuifen Xie
Surface defects on electrocatalysts can effectively reduce reaction barriers and facilitate the kinetics of hydrogen evolution and oxidation reactions (HER/HOR). However, precisely engineering such surface structures remains a significant challenge. Herein, penta-twinned (PTw) Rh@Pt x core–shell nanobranches (NBs) with intense surface strains were facilely synthesized using PTw Rh NBs as the seeds for overgrowth of active Pt-shells. Through precisely regulating the supply of Pt precursor solution via a micro-syringe pump, the ultrathin Pt-shells conform to and replicate the twin defects of the PTw Rh seeds. Significantly, the shell thickness can be precisely controlled from 1.0, 2.0, and 3.8 to 5.0 atomic layers. Due to the integration of surface twinned defects, compressive strain and the core–shell ligand effect, these Rh@Pt x NBs exhibit superior hydrogen redox electrocatalytic performance compared to state-of-the-art Pt/C. Among the prepared materials, the Rh@Pt 0.83 NBs with a 3.8 atomic layer Pt-shell showed the highest mass activity (2.36 A mg Pt −1 ) and specific activity (6.55 mA cm −2 ) for HER at –0.07 V and presented the lowest overpotential (44 mV) at 10 mA cm −2 , less than half the overpotential of the commercial Pt/C (98 mV). In terms of HOR, the Rh@Pt 0.83 NBs showed a superior exchange current density (1.97 mA cm −2 ), approximately 7 times higher than that of Pt/C. Our work provides a facile method to synchronously engineer the Pt-shell thickness and surface defects of Rh@Pt core–shell nanocatalysts for the creation of robust and bifunctional hydrogen redox electrocatalysts.
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BIOSENSORS & BIOELECTRONICS
·
2021
·
IF 10.618
Qilin Li,Yan Zhang,Huiling Fan,Yuji Gong,Yun Xu,Qiying Lv,Yunruo Xu,Fei Xiao,Shuai Wang,Zheng Wang,Lin Wang
Accelerated glucose uptake and “aerobic glycolysis” of tumor cells generates a high-level lactate in extracellular space and within tumor tissue, which is thought to be a hallmark of tumor and closely correlated with tumor development. Here, we report the development of an enzyme-free electrochemical sensing platform based on a Pt-microneedle electrode functionalized with Au nanoparticles (Au-NPs) decorated polydopamine nanospheres (PDA-NSs), and explore its practical application in in vitro and in vivo detection of lactate in different biological samples. Our results demonstrate that in virtue of the nanostructured merits and high electrocatalytic activity , the resultant nanohybrid-microelectrode exhibits good sensitivity and selectivity to the nonenzymatic electrochemical detection of lactate, with a detection limit of 50 μM, a liner range of 0.375–12 mM, and a sensitivity of 11.25 mA mM −1 cm −2 , as well as a good anti-interference ability to other active small molecules . The platform quantifies lactate in complex bio-fluids, including cancerous and non-cancerous cell culture media, as well as serum samples, with detecting time 7.5-fold faster than does a clinically-used approach. Moreover, owing to miniaturized size and satisfactory electrochemical performance, the sensor achieves in vivo recording of lactate-related characteristic voltammetric signals within a living tumor, which are positively correlated with tumor burden and growth. Therefore, the platform cannot only be employed for cancer metabolic investigation, but also potentially for clinical assessment of tumor progression, and even clinical diagnosis of other lactate metabolism disorders.
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PubMed
高影响因子
ACS Applied Energy Materials
·
2021
·
IF 6.024
Dewei Yao,Hongmei Yu,Wei Song,Xueqiang Gao,Xinye Sun,Guang Jiang,Jinkai Hao,Zhigang Shao
To reduce cost and energy consumption of fuel cell vehicles, constructing membrane electrode assemblies (MEAs) with low Pt loading and outstanding performance at low relative humidity (RH) conditions is reported. A catalyst layer based on porous Pt–Ni nanobelt arrays was prepared, in which the strained catalyst enhanced the catalytic activity and the oriented nanobelt array structure provided convenient mass transport channels. The porous Pt–Ni nanobelt arrays were prepared by the magnetron sputtering of Pt and Ni on a sacrificed template and then washed with acid. Consequently, the catalyst layer based on the porous Pt–Ni nanobelt arrays exhibited superior fuel cell performance in H2/air conditions and RH 40%. The performance of the MEA with porous Pt–Ni nanobelt arrays reach 366.6 and 597.6 mW cm–2 with Pt loadings of 36.5 μg cm–2/36.5 μg cm–2 and 108.9 μg cm–2/108.9 μg cm–2 at the cathode/anode, respectively. A conventional CCM with the Pt loading of 100 μg cm–2/200 μg cm–2 at the cathode/anode served as the benchmark, and the cell performance was 230.5 mW cm–2. Apart from that, the Pt nanobelt arrays without a porous structure (100.8 g cmPt–2/100.8 μg cmPt–2) serving as another benchmark achieved a performance of 504.7 mW cm–2. The superior performance of the porous Pt–Ni nanobelt arrays is attributed to the convenient mass transport pathway and the high activity of the porous Pt–Ni nanobelt.
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Solar RRL
·
2021
·Vol. 5
·期 11
·2100536
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IF 8.582
Yujie Liu,Qiaohong Zhu,Muhammad Tayyab,Liang Zhou,Juying Lei,Jinlong Zhang
Semiconductor supported noble metal nanoparticles are widely used in H 2 evolution. Due to the high cost and low catalytic efficiency of noble metals, single-atom catalysts (SACs) are considered as very potential materials to overcome these shortcomings. Herein, the construction of the ZnO–ZnS heterojunction with an excess amount of Zn vacancies promotes the separation of charge carriers and improves the utilization of electrons. Meanwhile, the zinc vacancies on ZnS provide effective anchor sites for Pt atoms, which is beneficial to obtain highly dispersed single Pt atoms catalyst (ZOS-SAPt). Due to the formation of an intermediate energy level by zinc vacancies, the introduction of Pt single atoms promotes the novel type-V electron transport from the conduction band of ZnO to the intermediate energy level and then to the Pt atom. The type-V electron transport not only retains the high reduction potential of photogenerated electrons, but also avoids the loss of carriers. The resultant ZOS-SAPt shows outstanding photocatalytic performance for H 2 evolution under simulated sunlight, reaching 9.6 mmol g −1 h −1 , which is 201 times that of ZnO–ZnS. These results provide important information for further development of photocatalysts.
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NANOTECHNOLOGY
·
2019
·Vol. 30
·期 49
·495706
·
IF 3.399
Jianghua Yang,Cong Luo,Shijie He,Jinling Li,Bowen Meng,Dongxia Zhang,Zhonghua Xue,Xibin Zhou,Xiaoquan Lu
Au-graphene quantum dots (GQDs)@Pt core–shell nanodendrites are synthesized through a two-step reduction approach, in which Au forms the core, GQDs form an intermediate layer and dendritic Pt forms the shell. Among the above synthesized catalysts, the GQDs can manipulate the binding of reaction intermediates on the Pt surface as well as assemble π–π* conjugate bonds, thus forming a dendritic Pt shell instead of a compact Pt shell. The obtained core–shell structure was characterized by transmission electron microscopy, energy-dispersive x-ray and x-ray photoelectron spectroscopy. The methanol electro-oxidation was investigated in alkaline media on the Au-GQDs@Pt modified electrode via cyclic voltammetry, chronoamperometry and electrochemical impedance spectroscopy analysis. In particular, we discovered that Au–Pt assembled with GQDs could dramatically improve the activity and stability of the catalysts, owing to the synergistic effect raised by the GQDs, which exhibit prominent electron conductivity and great chemical/physical stability. It was also found that the Pt/Au mole ratios could control the Pt shell thickness, which significantly affected the catalytic methanol oxidation activity of the Au-GQDs@Pt nanodendrites. The Au-GQDs@Pt nanodendrites with optimum Pt/Au mole ratios of 1.0 exhibited a 2.5 times increase in electrocatalytic activity toward methanol oxidation compared with the commercial catalyst (Pt/C), and its CO tolerance was also greatly improved. The above results show that the Au-GQDs@Pt nanocatalysts have potential application prospects in direct methanol fuel cells.
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PubMed
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Nano Research
·
2020
·Vol. 13
·期 1
·160-172
·
IF 8.183
Zhang Amin,Zhang Qian,Alfranca Gabriel,Pan Shaojun,Huang Zhicheng,Cheng Jin,Ma Qiang,Song Jie,Pan Yunxiang,Ni Jian,Ma Lijun,Cui Daxiang
Distinctively different metabolism between tumor cells and normal cells endows tumor tissues unique microenvironment. In this regard, we have successfully prepared a sequential catalytic platform based on Au/Pt star for tumor theragnostic. The multifunctional probes consisted of a gold/platinum star-shaped core (Au/Pt star) conjugated with a GSH-sensitive disulfide bond (S–S), a targeting ligand (rHSA-FA), a near-infrared fluorophore (IR780) and glucose oxidase (GO x ). When systemically administered in a xenografted murine model, the probes specifically targeted the tumor sites. As the disulfide linker was cleaved by intracellular GSH, the IR780 molecules could be released for photo-thermal therapy & photodynamic therapy (PTT&PDT) and imaging. Subsequently, the Pt nanolayer of the Au/Pt star and the GO x formed a sequential catalytic system: GO x effectively catalyzed intracellular glucose by consuming oxygen to generate H 2 O 2 and enhance the local acidity, and the Pt layer exhibited peroxidase-like property to catalyze H 2 O 2 producing toxic ·OH for tumor oxidative damage. Here we demonstrated that our probes simultaneously possessed a GSH-sensitive release, real-time imaging ability, and synergetic cancer starving-like therapy/enzyme oxidative therapy/PTT/PDT features, which provides a potential strategy for effective tumor theragnostic.
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ANALYTICA CHIMICA ACTA
·
2020
·
IF 5.977
Meng Li,Jie Lv,Shuangling Wang,Jing Wang,Yulong Lin
Design of synthetic structures that possess the similar functions to natural enzymes held great promise in environmental detection and biomedical application. Herein, a new concept for the fabrication of solid-supported catalysts as peroxidase mimic have been proposed to realize high-catalytic activity and stability by utilizing expanded mesoporous silica (EMSN)-encapsulated Pt nanoclusters . Compared with PtNCs, the introduction of amino group modified EMSN would enrich H 2 O 2 on the surface of PtNCs and increase the catalytic sites for H 2 O 2 decomposition, which gave rise to the higher catalytic activity of EMSN-PtNCs over a broad pH range, especially in weakly acidic and neural solutions. This would facilitate their applications for real-time monitoring the secretion of H 2 O 2 from living cancer cells stimulated by various anticancer drugs . Our findings not only pave the way to use porous matrix as the structural component for the design of the biomimetic catalysts , but also provide a simple and reliable platform to monitor H 2 O 2 released from living cells in real time, which holds great potential for elucidating the biological roles of H 2 O 2 and underlying molecular mechanisms of drug cytotoxicity as well as drug therapeutic effects.
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PubMed
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Nanoscale
·
2019
·Vol. 11
·期 18
·9091-9102
·
IF 6.97
Dahui Fang,Xuejun Tang,Limeng Yang,Dongyan Xu,Hongjie Zhang,Shucheng Sun,Zhigang Shao,Baolian Yi
Pt-Decorated Ir black (Pt@Ir) nanoparticles with two varying Pt mass fractions (Pt4@Ir96 and Pt16@Ir84) were generated by a facile method in water with the aid of Ir black. The Pt@Ir nanoparticles were investigated as a bifunctional oxygen catalysts for both the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) in acidic medium. Benefiting from the good dispersion of ultrafine Pt nanodots on the Ir black surface and the synergistic effect between the Pt and underlying Ir atoms, Pt@Ir nanoparticles have exhibited outstanding ORR activity and comparable OER performance in comparison with commercial Ir black. In particular, Pt16@Ir84 shows an ORR mass activity of 2.6 times that of commercial Pt black and exhibits much better bifunctional performances than a mixture of Pt black and Ir black with a Ir/Pt mass ratio of 50/50 (Pt50Ir50). Our work highlights the effectiveness of decorating Ir black with Pt nanodots to fabricate bifunctional oxygen catalysts.
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PubMed
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2019
·
IF 4.175
Kaifeng Zhao,Xue Zhang,Mingkun Wang,Wenming Zhang,Xiaoting Li,Hongjie Wang,Ling Li
Carbon nanofibers (CNs) supported by Pt and Ni 2 P nanoparticles (Pt-Ni 2 P/CNs) are successfully synthesized and explored as counter electrodes for dye-sensitized solar cells (DSSCs) for the first time. Pt and Ni 2 P nanoparticles are prepared by stabilization and carbonization of electrospun nanofibers , and subsequently controllable Pt and Ni 2 P nanoparticles are grown on surface of CNs obtained through redox reaction . A series of electrochemical measurements analysis confirm that the Pt-Ni 2 P/CNs composite have simultaneously superior electrocatalytic activity and enhanced electrical conductivity compared with those of individual CNs and Pt. Accordingly, DSSCs using the composite Pt-Ni 2 P/CNs as a counter electrode exhibit an excellent photovoltaic performance (power conversion efficiency of 9.11%), which is much higher than conventional Pt/CNs counter electrode (power conversion efficiency of 8.35%), owing to the collective effect of the high electrical conductivity originated from carbon nanofibers and superior electrocatalytic activity arising from Pt/CNs nanoparticles.
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ELECTROCHIMICA ACTA
·
2019
·
IF 5.383
Li Ma,Ying He,Youran Wang,Yuhua Wang,Ruotong Li,Zhihong Huang,Yanjun Jiang,Jing Gao
Pt nanoparticle-anchored zirconium-based metal organic framework nanocomposites (Pt@UiO66-NH 2 ) with large surface areas and highly dispersed Pt nanoparticles were synthesized and applied to prepare acetylcholinesterase (AChE) biosensors for organophosphorus pesticides (OPs) detection. Because of integrative impact of excellent electron conduction channels and the increasing of adsorption sites of Pt@UiO66-NH 2 as well as the ultrahigh surface area to increase AChE immobilization, the prepared biosensors exhibited high sensitivity towards malathion (as a model for OPs), malathion was detected ranging from 1 × 10 −14 M to 1 × 10 −9 M and 4.9 × 10 −15 M was regarded as limit of detection. The biosensors also displayed accurately. Moreover, the Pt@UiO66-NH 2 /GCE was used to detect OPs in cabbage and apple samples. This study manifests the profound potential of metal nanoparticle/MOF composites for biosensors with improved electrochemical performance.
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高影响因子
NANO
·
2019
·
IF 1.293
Yunong Zhou,Chao Hu,Weidong Zhang,Hong Chen,Gang Yu
The ability to control the shape, structure and faceting characteristics of bimetallic alloy nanocrystals (NCs) has been vital for designing a catalyst with excellent activity and durability in fuel cells. However, it has remained a significant challenge to synthesize platinum–copper (Pt–Cu) alloy NCs with controlled structure and exposed facets. Herein, Pt–Cu alloy NCs with different shapes, structures and facets were synthesized via a one-step direct chemical co-reduction method employing various glucose concentrations. The results showed that the prepared Pt–Cu alloy NCs exhibited very interesting facet-dependent electrocatalytic properties for ethylene glycol oxidation. In comparison with other prepared Pt–Cu alloy NCs and commercial Pt/C, Pt–Cu alloy NPs with (111)-dominant facets showed higher electrocatalytic activity and durability for ethylene glycol oxidation. Alloy NPs showing prominent electrocatalytic performance were attributed to the predominant (111) facets on NP surfaces serving as catalytic active sites, in addition to added Cu providing unique electronic and synergistic effects. The present work highlighted that these NPs with (111)-dominant facets were indeed promising candidates as electrocatalysts with excellent activity and superior durability.
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危险品化学品经营许可证（带存储）