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16. Diamond for biosensor applications

Author

Nebel, Christoph E., Rezek, Bohuslav, Shin, Dongchan, Uetsuka, Hiroshi, and Yang, Nianjun

Subjects
Physics - Applied Physics, Condensed Matter - Materials Science
Abstract

A summary of photo- and electrochemical surface modifications applied on single-crystalline chemical vapor deposition (CVD) diamond films is given. The covalently bonded formation of amine- and phenyl-linker molecule layers are characterized using X-ray photoelectron spectroscopy (XPS), atomic force microscopy (AFM), cyclic voltammetry and field-effect transistor characterization experiments. Amine- and phenyl-layers are very different with respect to formation, growth, thickness and molecule arrangement. We detect a single molecular layer of amine linker-molecules on diamond with a density of about 1014 cm-2 (10 % of carbon bonds). Amine molecules are bonded only on initially H-terminated surface areas to carbon. In case of electrochemical deposition of phenyl-layers, multi-layer formation is detected due to three dimensional (3D) growths. This gives rise to the formation of typically 25 {\AA} thick layers. The electrochemical grafting of boron doped diamond works on H-terminated and oxidized surfaces. After reacting of such films with heterobifunctional crosslinker-molecules, thiol-modified ss-DNA markers are bonded to the organic system. Application of fluorescence and atomic force microscopy on hybridized DNA films show dense arrangements with densities up to 1013 cm-2. The DNA is tilted by an angle of about 35o with respect to the diamond surface. Shortening the bonding time of thiol-modified ss-DNA to 10 minutes cause a decrease of DNA density to about 1012 cm-2. Application of AFM scratching experiments show threshold removal forces around 75 nN for DNA bonded on phenyl linker-molecules and of about 45 nN for DNA bonded to amine linker-molecules. DNA sensor applications using Fe(CN6)3-/4- mediator redox-molecules, impedance spectroscopy and DNA-field effect transistor devices performances are introduced and discussed.

Published
2020
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25. Battery-like Supercapacitors from Vertically Aligned Carbon Nanofibers Coated Diamond: Design and Demonstrator

Author

Yu, Siyu, Yang, Nianjun, Vogel, Michael, Mandal, Soumen, Williams, Oliver A., Jiang, Siyu, Schönherr, Holger, Yang, Bing, and Jiang, Xin

Subjects
Physics - Applied Physics, Condensed Matter - Materials Science
Abstract

Battery-like supercapacitors feature high power and energy densities as well as long-term capacitance retention. The utilized capacitor electrodes are thus better to have large surface areas, high conductivity, high stability, and importantly be of binder free. Herein, vertically aligned carbon nanofibers (CNFs) coated boron-doped diamonds (BDD) are employed as the capacitor electrodes to construct battery-like supercapacitors. Grown via a thermal chemical vapor deposition technique, these CNFs/BDD hybrid films are binder free and own porous structures, resulting in large surface areas. Meanwhile, the containment of graphene layers and copper metal catalysts inside CNFs/BDD leads to their high conductivity. Electric double layer capacitors (EDLCs) and pseudocapacitors (PCs) are then constructed in the inert electrolyte (1.0 M H2SO4 solution) and in the redox-active electrolyte (1.0 M Na2SO4 + 0.05 M Fe(CN)63-/4-), respectively. For assembled two-electrode symmetrical supercapacitor devices, the capacitances of EDLC and PC devices reach 30 and 48 mF cm-2 at 10 mV s-1, respectively. They remain constant even after 10 000 cycles. The power densities are 27.3 kW kg-1 and 25.3 kW kg-1 for EDLC and PC devices, together with their energy densities of 22.9 Wh kg-1 and 44.1 Wh kg-1, respectively. The performance of formed EDLC and PC devices is comparable to market-available batteries. Therefore, the vertically aligned CNFs/BDD hybrid film is a suitable capacitor electrode material to construct high-performance battery-like and industry-orientated supercapacitors for flexible power devices.

Published
2018
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34. Construction and Progress of Small Molecule‐Based Coupled Electrolyzers.

Author

Qin, Yanxi, Wang, Yingyong, Jin, Guoqiang, Tong, Xili, and Yang, Nianjun

Abstract

Coupled electrolyzer is a desirable way to realize efficient energy conversion from electricity to chemical energy. Using coupled electrolyzers highly valuable chemicals (e.g., H2, CHxCOO−, nitrile, S, NH3, CO) can be obtained at low voltages, environmental pollutants can be alleviated, and wastewater (e.g., ammonia, urea, hydrazine) can be recycled. They are even helpful to realize the goal of carbon peaking and carbon neutrality. Compared to traditional chemical methods, small molecule‐based coupled electrolyzers are more cost‐efficient. This review summarizes state‐of‐art of coupled electrolyzers, mainly the replacement of oxygen reduction reaction with oxidation reactions of small molecules and their further coupling with cathodic reduction reactions such as hydrogen evolution reaction (HER), oxygen reduction reaction (ORR), CO2 reduction reaction (CO2RR), N2 reduction reaction (NRR), and other reduction reactions of matching small molecules. In terms of oxidation reactions of small molecules, two types of reactions are covered: sacrificial agent oxidation reaction (SAOR) and electrochemical synthesis reaction (ESR). After detailing the design principle of coupled electrolyzers and several oxidation reactions of small molecules, construction, characterization, and performance of coupled electrolyzers are systematically overviewed along with discussion and outline of current challenges and prospects of this appealing strategy. [ABSTRACT FROM AUTHOR]

Published
2024
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44. Nitrogen-containing Carbonaceous Materials for Electrochemical Oxygen Reduction Reaction

Author

Raoux, Simone, Koch, Norbert, Yang, Nianjun, Wu, Bin, Raoux, Simone, Koch, Norbert, Yang, Nianjun, and Wu, Bin

Abstract

Der steigende weltweite Energiebedarf treibt die Entwicklung sauberer Energiequellen voran, die dazu beitragen werden, den Verbrauch fossiler Brennstoffe zu reduzieren. Brennstoffzellen und Metall-Luft-Batterien sind vielversprechende Alternativen, um traditionelle fossile Energie zu ersetzen und durch die Reduzierung von O2 an der Kathode grünen Strom zu erzeugen. Aufgrund der langsamen Reaktionsraten der Sauerstoffreduktionsreaktion (ORR) ist hierfür jedoch elektrokatalytisches Material mit geringen Kosten und hoher Effizienz erforderlich. In den letzten Jahrzehnten wurde eine Vielzahl von Materialien als Nicht-Pt-Katalysatoren getestet, von metallfreien Katalysatoren bis hin zu Katalysatoren auf Übergangsmetallbasis. Aufgrund des mangelnden Verständnisses des Reaktionsmechanismus und der Wechselwirkung zwischen Elektrolyt und Elektrokatalysator befinden sich neue Designs stickstoffhaltiger Katalysatoren auf Kohlenstoffbasis jedoch noch in der Entwicklungsphase. Zu diesem Zweck wurden verschiedene (in situ) spektroskopische und elektrochemische Techniken eingesetzt, um die Wechselwirkung zwischen N-dotiertem Kohlenstoff und Elektrolyten sowie die katalytischen Mechanismen zu verstehen. Darüber hinaus weisen die neu entwickelten Katalysatoren für die ORR eine überlegene elektrokatalytische Leistung auf, die in dieser Dissertation ausführlich diskutiert wird. Die Struktur-Leistungs-Beziehung unserer ORR-N-dotierten Kohlenstoffkatalysatoren wurde gründlich untersucht. Diese Forschung zeigt, wie die Kombination fortschrittlicher Spektroskopietechniken, einschließlich In-situ-Spektroskopie und elektrochemischer Charakterisierung, ein tieferes Verständnis der Katalysator-/Elektrolyt-Wechselwirkung, des katalytischen Mechanismus und der optimierten elektrokatalytischen Leistung stickstoffhaltiger Kohlenstoffmaterialien, ORR-Katalysatoren, insbesondere nanoporöser N-dotierter Kohlenstoff, fördern kann Eisen-Stickstoff-codotierte Kohlenstoffmaterialien., Increasing global energy demand drives the development of clean energy sources that will help reduce the consumption of fossil fuels. Fuel cells and metal-air batteries are promising alternatives to replace traditional fossil energy to generate green electricity by reducing O2 at the cathode. However, due to sluggish reaction rates of oxygen reduction reaction (ORR), this requires electrocatalytic material with low cost and high efficiency. Over the last few decades, a variety of materials have been tested as non-Pt catalysts, from metal-free catalysts to transition metal-based catalysts. However, due to the lack of understanding of the reaction mechanism and the interaction between electrolyte and electrocatalysts, new designs nitrogen-containing carbon-based catalysts are still under the development stage. To this aim, a variety of (in situ) spectroscopic and electrochemical techniques to understand N-doped carbon electrocatalysts/electrolyte interaction and catalytic mechanisms have been employed. Moreover, the newly-designed catalysts for ORR demonstrate superior electrocatalytic performance which are discussed in detail in this dissertation. The structure-performance relationship for our ORR N-doped carbon catalysts has been thoroughly investigated. This research highlights how the combination of advanced spectroscopy techniques including in situ spectroscopy and electrochemical characterization may promote a deeper understanding of catalyst/electrolyte interaction, catalytic mechanism and optimized electrocatalytic performance of nitrogen-containing carbon materials ORR catalysts, especially nanoporous N-doped carbon and iron-nitrogen-co-doped carbon materials.

Published
2024

45. Diamond Nanostructures at Different Dimensions: Synthesis and Applications.

Author

Li, Yao, Yang, Limin, Jiang, Xin, Lu, Yang, Han, Cuiping, Tang, Yongbing, and Yang, Nianjun

Subjects
NANODIAMONDS, ELECTRON field emission, DIAMONDS, YOUNG'S modulus, NANOSTRUCTURES, ELASTICITY
Abstract

Diamond materials at different nanoscales provide them various characteristics such as elastic mechanical properties in needle‐like nanotips, flexibility of 2D films having atomic thicknesses and constant hardness under high pressures, superior field electron emission properties of vertically wall‐like composites, unprecedented hardness and improved toughness of nanotwin diamond (nt‐diamond), while the inherent excellent properties of bulk diamond (e.g., high Young's modulus, robustness, biocompatibility) can be maintained. In this paper, the newly born 1D diamond nanothreads, 2D diamanes, as well as 3D nt‐diamond are briefly reviewed. The innovations, progresses and achievements of different dimensional diamond nanostructures, covering lines, planes and volumes are overviewed. The topical problems and future outlooks of diamond nanostructures are outlined and discussed. [ABSTRACT FROM AUTHOR]

Published
2024
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