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Sharifi, T., Gracia-Espino, E., Chen, A., Hu, G. & Wågberg, T. (2019). Oxygen Reduction Reactions on Single- or Few-Atom Discrete Active Sites for Heterogeneous Catalysis. Advanced Energy Materials, Article ID 1902084.
Open this publication in new window or tab >>Oxygen Reduction Reactions on Single- or Few-Atom Discrete Active Sites for Heterogeneous Catalysis
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2019 (English)In: Advanced Energy Materials, ISSN 1614-6832, article id 1902084Article in journal (Refereed) Epub ahead of print
Abstract [en]

The oxygen reduction reaction (ORR) is of great importance in energy-converting processes such as fuel cells and in metal-air batteries and is vital to facilitate the transition toward a nonfossil dependent society. The ORR has been associated with expensive noble metal catalysts that facilitate the O-2 adsorption, dissociation, and subsequent electron transfer. Single- or few-atom motifs based on earth-abundant transition metals, such as Fe, Co, and Mo, combined with nonmetallic elements, such as P, S, and N, embedded in a carbon-based matrix represent one of the most promising alternatives. Often these are referred to as single atom catalysts; however, the coordination number of the metal atom as well as the type and nearest neighbor configuration has a strong influence on the function of the active sites, and a more adequate term to describe them is metal-coordinated motifs. Despite intense research, their function and catalytic mechanism still puzzle researchers. They are not molecular systems with discrete energy states; neither can they fully be described by theories that are adapted for heterogeneous bulk catalysts. Here, recent results on single- and few-atom electrocatalyst motifs are reviewed with an emphasis on reports discussing the function and the mechanism of the active sites.

Place, publisher, year, edition, pages
WILEY-V C H VERLAG GMBH, 2019
Keywords
active sites, catalyst motifs, electrocatalysis, oxygen reduction reaction, single active atom catalysts, transition metals, X-ray adsorption spectroscopy
National Category
Other Chemistry Topics
Identifiers
urn:nbn:se:umu:diva-164137 (URN)10.1002/aenm.201902084 (DOI)000486795700001 ()
Available from: 2019-10-17 Created: 2019-10-17 Last updated: 2019-10-17
Sukhrobov, P., Numonov, S., Liu, J., Luo, J., Mamat, X., Li, Y., . . . Hu, G. (2019). Rapid Microwave-Assisted Synthesis of Copper Decorated Carbon Black Nanocomposite for Non-Enzyme Glucose Sensing in Human Blood. Journal of the Electrochemical Society, 166(13), B1238-B1244
Open this publication in new window or tab >>Rapid Microwave-Assisted Synthesis of Copper Decorated Carbon Black Nanocomposite for Non-Enzyme Glucose Sensing in Human Blood
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2019 (English)In: Journal of the Electrochemical Society, ISSN 0013-4651, E-ISSN 1945-7111, Vol. 166, no 13, p. B1238-B1244Article in journal (Refereed) Published
Abstract [en]

The current research performs the novelty fabricated of non-enzymatic biosensor based on copper nanoparticles decorated carbon black nanocomposite modified glassy carbon electrode (Cu/DCB/GCE) by using the microwave method. The prepared nanomaterial was applied for glucose determination in biological fluids and human serum samples. The techniques of SEM, TEM, XPS, XRD, EDS and mapping tests were selected for the morphological, compositions and crystal structure characterizations of the fabricated nanocomposite. In comparison with other electrodes based on metal decorated carbon black, the Cu/DCB/GCE demonstrated the best electrocatalytic property toward glucose oxidation in 0.1 M KOH electrolyte. Cu/DCB/GCE under the optimal potential of +0.5 V in a linear range from 0.5 up to 7000 mu M with a detection limit of 0.1 mu M (S/N=3), the coefficient of correlation R-2=0.999, performed significant high sensitivity of 1595 mu A mM(-1) cm(-2). Rapid amperometric responses of the prepared biosensor in short time with 0.8-2 s were observed by addition of different glucose concentrations in alkaline solution. Modified Cu/DCB/GCE exhibited the best anti-interference property against blood cells and some blood co-existence molecules such as dopamine, uric acid, ascorbic acid, albumin, and globulin. Most importantly, Cu/DCB/GCE biosensor was used for glucose level determination in human blood serum samples. Due to the attractable structure and properties of the fabricated biosensor, it can be suggested for the future development of glucose detection design.

Place, publisher, year, edition, pages
Electrochemical Society, 2019
National Category
Analytical Chemistry Materials Chemistry
Identifiers
urn:nbn:se:umu:diva-164407 (URN)10.1149/2.0011914jes (DOI)000485886400001 ()
Available from: 2019-11-05 Created: 2019-11-05 Last updated: 2019-11-05Bibliographically approved
Han, X.-B., Tang, X.-Y., Lin, Y., Gracia-Espino, E., Liu, S.-G., Liang, H.-W., . . . Zheng, L.-S. (2019). Ultrasmall Abundant Metal-Based Clusters as Oxygen-Evolving Catalysts. Journal of the American Chemical Society, 141(1), 232-239
Open this publication in new window or tab >>Ultrasmall Abundant Metal-Based Clusters as Oxygen-Evolving Catalysts
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2019 (English)In: Journal of the American Chemical Society, ISSN 0002-7863, E-ISSN 1520-5126, Vol. 141, no 1, p. 232-239Article in journal (Refereed) Published
Abstract [en]

The oxygen evolution reaction is a crucial step in water electrolysis to develop clean and renewable energy. Although noble metal-based catalysts have demonstrated high activity for the oxygen evolution reaction, their application is limited by their high cost and low availability. Here we report the use of a molecule-to-cluster strategy for preparing ultrasmall trimetallic clusters by using the polyoxometalate molecule as a precursor. Ultrafine (0.8 nm) transition-metal clusters with controllable chemical composition are obtained. The transition-metal clusters enable highly efficient oxygen evolution through water electrolysis in alkaline media, manifested by an overpotential of 192 mV at 10 mA cm–2, a low Tafel slope of 36 mV dec–1, and long-term stability for 30 h of electrolysis. We note, however, that besides the excellent performance as an oxygen evolution catalyst, our molecule-to-cluster strategy provides a means to achieve well-defined transition-metal clusters in the subnanometer regime, which potentially can have an impact on several other applications.

Place, publisher, year, edition, pages
American Chemical Society (ACS), 2019
National Category
Materials Chemistry
Identifiers
urn:nbn:se:umu:diva-155964 (URN)10.1021/jacs.8b09076 (DOI)000455561800040 ()30540181 (PubMedID)
Funder
Carl Tryggers foundation , CTS-16-161
Available from: 2019-02-07 Created: 2019-02-07 Last updated: 2019-02-07Bibliographically approved
Sukhrobov, P., Numonov, S., Mamat, X., Li, Y., Wågberg, T. & Hu, G. (2018). A New Non-Enzymatic Amperometric Sensor Based on Nickel Decorated ZIF-8 Derived Carbon Nanoframe for the Glucose Determination in Blood Samples. International Journal of Electrochemical Science, 13(7), 6550-6564
Open this publication in new window or tab >>A New Non-Enzymatic Amperometric Sensor Based on Nickel Decorated ZIF-8 Derived Carbon Nanoframe for the Glucose Determination in Blood Samples
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2018 (English)In: International Journal of Electrochemical Science, ISSN 1452-3981, E-ISSN 1452-3981, Vol. 13, no 7, p. 6550-6564Article in journal (Refereed) Published
Abstract [en]

The present study demonstrated a highly sensitive non-enzymatic glucose biosensor in real blood samples based on simple evaluated nickel deposited on N-doped porous carbon modified glassy carbon electrode (Ni/NPC/GCE) by applying electrochemical deposition method. The prepared material initially were characterized by cyclic voltammetry, the morphology structure of the as-prepared samples was observed by SEM, and composition, crystals structure of Ni/NPC were identified by SEM mapping and EDS tests. The Ni/NPC/GCE compared with NPC/GCE and NiNPs/GCE performed the best electrocatalytic behavior towards oxidation of glucose in 0.1 M KOH medium. By applied potential of +0.6 V Ni/NPC/GCE showed very high sensitivity of 3753.78 mu AmM(-1)cm(-2) in linear range of 1-7940 mu M with the correlation coefficient of R-2=0.995. The linear ranges get views above the concentration up to 7940 mu M with the detection limit of 0.3 mu M (S/N= 3). Amperometric time responses of prepared electrode towards different glucose concentrations are 0.8-1.3s. Finally, several positive characteristics such as very high sensitivity, weak working potential, nice anti-interference properties, long stability, good selectivity, and comparison with some other non-enzymatic sensors Ni/NPC/GCE executed high sensitivity, low detection limit and wide linear range to glucose sensing, thus the selected electrode is supplying for future glucose level determination design.

Place, publisher, year, edition, pages
ESG, 2018
Keywords
Nickel deposition, N-doped porous carbon, electrodeposition, glucose biosensor
National Category
Analytical Chemistry
Identifiers
urn:nbn:se:umu:diva-151567 (URN)10.20964/2018.07.03 (DOI)000441819300030 ()
Funder
Swedish Research Council, 2013-5252
Available from: 2018-09-10 Created: 2018-09-10 Last updated: 2018-09-10Bibliographically approved
Qin, D., Hu, X., Dong, Y., Mamat, X., Li, Y., Wågberg, T. & Hu, G. (2018). An Electrochemical Sensor Based on Green gamma-AlOOH-Carbonated Bacterial Cellulose Hybrids for Simultaneous Determination Trace Levels of Cd(II) and Pb(II) in Drinking Water. Journal of the Electrochemical Society, 165(7), B328-B334
Open this publication in new window or tab >>An Electrochemical Sensor Based on Green gamma-AlOOH-Carbonated Bacterial Cellulose Hybrids for Simultaneous Determination Trace Levels of Cd(II) and Pb(II) in Drinking Water
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2018 (English)In: Journal of the Electrochemical Society, ISSN 0013-4651, E-ISSN 1945-7111, Vol. 165, no 7, p. B328-B334Article in journal (Refereed) Published
Abstract [en]

An eco-friendly gamma-AlOOH-carbonated bacterial cellulose (gamma-AlOOH-CBC) hybrids material was fabricated by simple pyrolysis and hydrothermal treatments. The obtained hybrids possess an intrinsic 3D nanofibrous structure decorated with chaff-like gamma-AlOOH particles. Owing to the good adsorption property and conductive, gamma-AlOOH-CBC hybrids were used to modified the glass carbon electrode (GCE) for simultaneous determination of Cd(II) and Pb(II) in aqueous samples by differential pulse anodic stripping voltammetry (DPASV) method. Various parameters affected Cd(II) and Pb(II) measurement were optimized. Under the optimal conditions, the limit of detection (S/N = 3) of the gamma-AlOOH-CBC modified electrode was evaluated to be 0.17 mu g.L-1 for Cd(II) and 0.10 mu g.L-1 for Pb(II) with the linear range of the calibration curves ranged 0.5-250 mu g.L-1 for Cd(II) and Pb(II). Furthermore, the developed electrode was also successfully utilized for monitoring trace Cd(II) and Pb(II) in drinking water samples with satisfactory results.

Place, publisher, year, edition, pages
ELECTROCHEMICAL SOC INC, 2018
National Category
Materials Chemistry
Identifiers
urn:nbn:se:umu:diva-151076 (URN)10.1149/2.1321807jes (DOI)000440912000057 ()
Available from: 2018-08-27 Created: 2018-08-27 Last updated: 2018-08-27Bibliographically approved
Yalikun, N., Mamat, X., Li, Y., Hu, X., Wågberg, T. & Hu, G. (2018). Bacterial cellulose-based three-dimensional carbon nanofibers for the sensitive and selective determination of uric acid. Science of Advanced Materials, 10(11), 1623-1629
Open this publication in new window or tab >>Bacterial cellulose-based three-dimensional carbon nanofibers for the sensitive and selective determination of uric acid
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2018 (English)In: Science of Advanced Materials, ISSN 1947-2935, E-ISSN 1947-2943, Vol. 10, no 11, p. 1623-1629Article in journal (Refereed) Published
Abstract [en]

In recent years, the interest in the optimization of novel nanomaterials for electrodes preparation has received tremendous attention. This article describe about develop an electrochemical sensor for to detect the uric acid (UA). Firstly, the sensing materials of carbon nanofibers (CNFs) were prepared through an economical approach under freeze-dried, mainly for CNFs were successfully synthesized through carbonized biomass green bacterial cellulose (BC) at 800 degrees C. The obtained CNFs were used to modify the glassy carbon electrode (GCE), and have an excellent electrochemical response towards the UA. Under the optimized condition, the current response of UA at the CNFs/GCE increased also the peak current linearly with the UA concentration, the limitation of detection (LOD) calculated as 0.29 mu M (S/N = 3), revealing the a high sensitivity and an broader analytical range of the as-prepared CNFs/GCE. Finally, the proposed electrochemical sensor can be used for detection of UA in human urine with the satisfactory result.

Place, publisher, year, edition, pages
American Scientific Publishers, 2018
Keywords
Bacterial Cellulose, Carbon Materials, Selective Determination, Uric Acid, Urine Sample
National Category
Materials Chemistry
Identifiers
urn:nbn:se:umu:diva-153650 (URN)10.1166/sam.2018.3360 (DOI)000449470400012 ()
Funder
Swedish Research Council, 2013-5252Knut and Alice Wallenberg Foundation
Available from: 2018-11-27 Created: 2018-11-27 Last updated: 2018-11-27Bibliographically approved
Sandström, R., Hu, G. & Wågberg, T. (2018). Compositional Evaluation of Coreduced Fe-Pt Metal Acetylacetonates as PEM Fuel Cell Cathode Catalyst. ACS Applied Energy Materials, 1(12), 7106-7115
Open this publication in new window or tab >>Compositional Evaluation of Coreduced Fe-Pt Metal Acetylacetonates as PEM Fuel Cell Cathode Catalyst
2018 (English)In: ACS Applied Energy Materials, ISSN 2574-0962, Vol. 1, no 12, p. 7106-7115Article in journal (Refereed) Published
Abstract [en]

Platinum iron nanoparticles were produced by solvothermal coreduction of organic Fe and Pt precursor compounds and supported on conventional Vulcan XC 72. Evaluation of oxygen reduction performance reveals a highly active surface with up to 5 times the specific activity of commercial Pt Vulcan measured in O-2-saturated 0.1 M HClO4. A particle size of 5.5 nm for the best performing sample, produced from an initial metal ratio of 1:1, provided 28% higher mass activity than the commercial reference. Membrane electrode assemblies, optimized for both H-2/O-2 and direct formic acid fuel cells, were produced, and the PEM fuel cell cathodic performance displayed results with similar enhancements as its ex situ measured mass activity, although a delamination of the catalyst layer from the membrane could be observed even when employing a hot-pressing procedure during MEA fabrication. Physical characterizations including X-ray photoelectron spectroscopy and in situ X-ray diffraction reveal oxidized states of Fe incorporated into the disordered face-centered cubic Pt nanoparticles, supported by composition-dependent morphological changes as observed by transmission electron microscopy. The provided insight into fuel cell performance as well as CO-oxidation attributes are expected to assist in selecting suitable applications and operating conditions for such FePt type nanoparticles.

Place, publisher, year, edition, pages
American Chemical Society (ACS), 2018
Keywords
platinum iron nanoparticles, proton exchange membrane fuel cell, oxygen reduction reaction, solvothermal coreduction, membrane electrode assembly, hydrogen energy
National Category
Materials Chemistry Inorganic Chemistry
Identifiers
urn:nbn:se:umu:diva-156900 (URN)10.1021/acsaem.8b01536 (DOI)000458706800053 ()
Funder
Swedish Research Council, 2017-04862Swedish Energy Agency, 45419-1
Available from: 2019-03-09 Created: 2019-03-09 Last updated: 2019-04-29Bibliographically approved
Liu, N., Mamat, X., Jiang, R., Tong, W., Huang, Y., Jia, D., . . . Hu, G. (2018). Facile high-voltage sputtering synthesis of three-dimensional hierarchical porous nitrogen-doped carbon coated Si composite for high performance lithium-ion batteries. Chemical Engineering Journal, 343, 78-85
Open this publication in new window or tab >>Facile high-voltage sputtering synthesis of three-dimensional hierarchical porous nitrogen-doped carbon coated Si composite for high performance lithium-ion batteries
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2018 (English)In: Chemical Engineering Journal, ISSN 1385-8947, E-ISSN 1873-3212, Vol. 343, p. 78-85Article in journal (Refereed) Published
Abstract [en]

Various kinds of efforts have been devoted to ameliorate the serious volume-expansion effect and low electron conductivity of silicon-based materials in lithium ion batteries. Here, we report a facile high voltage sputtering process to prepare three-dimensional hierarchical porous nitrogen-doped carbon coated Si microsphere to significantly improve the lithium storage performance. The structure and morphology of the as-obtained samples are characterized by X-ray diffraction, transmission electron microscope and scanning electron microscope. The results indicate that the as-prepared composite is composed of silicon nanoparticles (similar to 100 nm) coated with conductive thin carbon layer (similar to 8.5 nm). The composite shows excellent lithium storage performance with a reversible capacity of 1565 mAh g(-1) after 100 cycles at a current density of 0.5 A g(-1), as well as a long cycling performance at the high current density of 2 A g(-1). The facile preparation process and highly silicon-loading (similar to 78%) makes the prepared material be a great potential application in lithium-ion batteries.

Keywords
Three-dimensional hierarchical porous nitrogen-doped carbon, Silicon nanoparticles, High voltage uttering, Void space, Lithium-ion batteries
National Category
Materials Chemistry
Identifiers
urn:nbn:se:umu:diva-147423 (URN)10.1016/j.cej.2018.02.111 (DOI)000430269200010 ()
Available from: 2018-07-20 Created: 2018-07-20 Last updated: 2018-07-20Bibliographically approved
Qin, D., Wang, L., Gao, S., Wang, Y., Mamat, X., Li, Y., . . . Hu, G. (2018). N-Doped Hollow Porous Carbon Spheres/Bismuth Hybrid Film Modified Electrodes for Sensitive Voltammetric Determination of Trace Cadmium. Electroanalysis, 30(9), 1906-1912
Open this publication in new window or tab >>N-Doped Hollow Porous Carbon Spheres/Bismuth Hybrid Film Modified Electrodes for Sensitive Voltammetric Determination of Trace Cadmium
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2018 (English)In: Electroanalysis, ISSN 1040-0397, E-ISSN 1521-4109, Vol. 30, no 9, p. 1906-1912Article in journal (Refereed) Published
Abstract [en]

In this work, N-doped hollow porous carbon spheres (N-HPCSs) were synthesized by silicon dioxide template-assisted polybenzoxazine (PB) coating strategy. The prepared N-HPCSs have a smooth hollow ball structure surrounded by a well-defined porous shell. Combining with in-situ plating of Bi film, the N-HPCSs were further fabricated a sensitive electrochemical platform for determination trace levels of Cd(II) by differential pulse anodic stripping voltammetry (DPASV). Under the optimized conditions, the Bi-N-HPCSs based sensor displays a linear response to Cd(II) over the range of 0.5gL(-1) to 150gL(-1). Meanwhile, the limit of detection (LOD, S/N=3) is estimated to be around 0.16gL(-1) for Cd(II), which is 31 times lower than the safety values set by United States Environmental Protection Agency (EPA) for the drinking water. Moreover, the proposed method was successfully applied to detection of Cd(II) in tap water and lake water, and the analytical results of the presented method are agreed well with inductively coupled plasma-mass spectrometry (ICP-MS) data. Due to the excellent analytical performance, the fabricated electrode is promised for future development in monitoring of cadmium pollution in the environment.

Place, publisher, year, edition, pages
Wiley-VCH Verlagsgesellschaft, 2018
Keywords
N-doped hollow porous carbon spheres, bismuth film, differential pulse anodic stripping voltammetry, cadmium, tap water, lake water
National Category
Analytical Chemistry
Identifiers
urn:nbn:se:umu:diva-152258 (URN)10.1002/elan.201700839 (DOI)000443938300004 ()
Available from: 2018-10-03 Created: 2018-10-03 Last updated: 2018-10-03Bibliographically approved
Sukhrobov, P., Numonov, S., Gao, S., Mamat, X., Wågberg, T., Guo, Y., . . . Hu, G. (2018). Nonenzymatic Glucose Biosensor Based on NiNPs/Nafion/Graphene Film for Direct Glucose Determination in Human Serum. NANO, 13(7), Article ID 1850075.
Open this publication in new window or tab >>Nonenzymatic Glucose Biosensor Based on NiNPs/Nafion/Graphene Film for Direct Glucose Determination in Human Serum
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2018 (English)In: NANO, ISSN 1793-2920, Vol. 13, no 7, article id 1850075Article in journal (Refereed) Published
Abstract [en]

This study describes a type of novel nickel nanoparticles (NiNPs) decorated on Nafiongraphene composite film by using the electrochemical deposition method. It was used to fabricate electrochemical biosensors for sensitive nonenzymatic glucose detection. Compared with the Nafion-graphene film and NiNPs-modified glassy carbon electrode (NiNPs-GCE), the NiNPs/Nafion/graphene/GCE showed the best electrocatalytic activity towards glucose oxidation in alkaline medium. The NiNPs/Nafion/graphene/GCE at an applied potential of +0.55 V in a linear range of 1-200 mu M presented a high sensitivity of 3437.25 mu A center dot mM(-1) cm(-2) with coefficient of correlation R-2 = 0.999; and in a linear range of 200-10800 mu M it performed the best sensitivity of 2848.6 mu A center dot mM(-1) cm(-2) with coefficient of correlation R-2 = 0.995 towards glucose oxidation. For a concentration up to 200 mu M, a linear range was obtained with a limit of detection of 0.6 mu M (signal to noise = 3) and as much as 10 800 mu M with a limit of detection of 0.82 mu M (signal to noise = 3). The time of responses was about 1-1.5 s with the addition of 0.1-1 mM glucose. In addition, NiNPs/Nafion/graphene/GCE also has a high anti-interference ability toward common oxidative interfering species, such as uric acid, ascorbic acid and dopamine. More importantly, NiNPs/Nafion/graphene/GCE was successfully used for the determination of glucose concentration in human serum samples in comparison with a local hospital. The NiNPs/Nafion/graphene/GCE exhibited high sensitivity, low working potential, good stability, excellent electrical properties, enhanced selectivity and fast amperometric responses to glucose oxidation. Thus, as a nonenzymatic sensor, it is promising for future glucose determination development.

Keywords
Nickel nanoparticles, graphene, electrodeposition, nonenzymatic glucose sensor
National Category
Materials Chemistry
Identifiers
urn:nbn:se:umu:diva-150839 (URN)10.1142/S1793292018500753 (DOI)000440354000004 ()
Available from: 2018-09-04 Created: 2018-09-04 Last updated: 2018-09-04Bibliographically approved
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ORCID iD: ORCID iD iconorcid.org/0000-0003-0324-2788

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