Advanced Materials

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Promoted Glycerol Oxidation Reaction in an Interface‐Confined Hierarchically Structured Catalyst

2018-11-18T00:34:15+00:00November 17th, 2018|Categories: Publications|Tags: , |

The confinement of Pt nanosheets is realized in a vertically erected graphene array with hierarchically porous architecture to address the mass‐diffusion limitation in interface‐confined catalysis. Such a confined 3D catalyst exhibits a much stronger oxidation and CC bond cleaving ability for the glycerol oxidation reaction, leading to a superior mass activity and selectivity toward C1 products than commercial Pt/C catalysts. Abstract Confined catalysis in a 2D system is of particular interest owing to the facet control of the catalysts and the anisotropic kinetics of reactants, which suppress side reactions and improve selectivity. Here, a 2D‐confined system consisting of intercalated Pt nanosheets within few‐layered graphene is demonstrated. The strong metal–substrate interaction between the Pt nanosheets and the graphene leads to the quasi‐2D growth of Pt with a unique (100)/(111)/(100) faceted structure, thus providing excellent catalytic activity and selectivity toward one‐carbon (C1) products for the glycerol oxidation reaction. A hierarchically porous graphene architecture, grown on carbon cloth, is used to fabricate the confined catalyst bed in order to enhance the mass‐diffusion limitation in interface‐confined reactions. Owing to its unique 3D porous structure, this graphene‐confined Pt catalyst exhibits an extraordinary mass activity of 2910 mA mgPt−1 together with a formate selectivity of 79% at 60 °C. This paves the way toward rational designs of heterogeneous catalysts for energy‐related applications.

Published in: "Advanced Materials".

Electronic and Optical Properties of 2D Materials Constructed from Light Atoms

2018-11-18T00:34:12+00:00November 17th, 2018|Categories: Publications|Tags: |

2D materials constructed from boron, carbon, nitrogen, and oxygen atoms show a rich structural diversity. This makes possible engineering of their electronic and optical properties through a refined structural control. Abstract Boron, carbon, nitrogen, and oxygen atoms can form various building blocks for further construction of structurally well‐defined 2D materials (2DMs). Both in theory and experiment, it has been documented that the electronic structures and optical properties of 2DMs are well tunable through a rational design of the material structure. Here, the recent progress on 2DMs that are composed of B, C, N, and O elements is introduced, including borophene, graphene, h‐BN, g‐C3N4, organic 2D polymers (2DPs), etc. Attention is put on the band structure/bandgap engineering for these materials through a variety of methodologies, such as chemical modifications, layer number and atomic structure control, change of conjugation degree, etc. The optical properties, such as photoluminescence, thermoluminescence, single photon emission, as well as the associated applications in bioimaging and sensing, are discussed in detail and highlighted.

Published in: "Advanced Materials".

An Ambipolar Superconducting Field‐Effect Transistor Operating above Liquid Helium Temperature

2018-11-18T00:34:08+00:00November 17th, 2018|Categories: Publications|Tags: |

An ambipolar superconducting field‐effect transistor is developed using a strongly correlated molecular system laminated on a SiO2/Si substrate. The low‐temperature electronic state is fine tuned in the vicinity of the superconductor‐to‐Mott‐insulator transition, utilizing the negative pressure effect from the substrate, which allows a small dose of hole or electron injection by the SiO2 dielectric to control the superconductivity above 4.2 K. Abstract Superconducting (SC) devices are attracting renewed attention as the demands for quantum‐information processing, meteorology, and sensing become advanced. The SC field‐effect transistor (FET) is one of the elements that can control the SC state, but its variety is still limited. Superconductors at the strong‐coupling limit tend to require a higher carrier density when the critical temperature (T C) becomes higher. Therefore, field‐effect control of superconductivity by a solid gate dielectric has been limited only to low temperatures. However, recent efforts have resulted in achieving n‐type and p‐type SC FETs based on organic superconductors whose T C exceed liquid He temperature (4.2 K). Here, a novel “ambipolar” SC FET operating at normally OFF mode with T C of around 6 K is reported. Although this is the second example of an SC FET with such an operation mode, the operation temperature exceeds that of the first example, or magic‐angle twisted‐bilayer graphene that operates at around 1 K. Because the superconductivity in this SC FET is of unconventional type, the performance of the present device will contribute not only to fabricating SC circuits, but also to elucidating phase transitions

Published in: "Advanced Materials".

Lowering the Schottky Barrier Height by Graphene/Ag Electrodes for High‐Mobility MoS2 Field‐Effect Transistors

2018-11-18T00:34:06+00:00November 17th, 2018|Categories: Publications|Tags: , |

Contact resistance between the channel and electrodes in MoS2 devices is significantly reduced using a low work function metal (Ag) and graphene as an interfacial layer between MoS2 and Ag because the Schottky barrier height is lowered at the contacts. Using graphene/Ag contacts instead of Ti/Au improves the field‐effect mobility, on/off current ratio, and photoresponsivity of the devices. Abstract 2D transition metal dichalcogenides (TMDCs) have emerged as promising candidates for post‐silicon nanoelectronics owing to their unique and outstanding semiconducting properties. However, contact engineering for these materials to create high‐performance devices while adapting for large‐area fabrication is still in its nascent stages. In this study, graphene/Ag contacts are introduced into MoS2 devices, for which a graphene film synthesized by chemical vapor deposition (CVD) is inserted between a CVD‐grown MoS2 film and a Ag electrode as an interfacial layer. The MoS2 field‐effect transistors with graphene/Ag contacts show improved electrical and photoelectrical properties, achieving a field‐effect mobility of 35 cm2 V−1 s−1, an on/off current ratio of 4 × 108, and a photoresponsivity of 2160 A W−1, compared to those of devices with conventional Ti/Au contacts. These improvements are attributed to the low work function of Ag and the tunability of graphene Fermi level; the n‐doping of Ag in graphene decreases its Fermi level, thereby reducing the Schottky barrier height and contact resistance between the MoS2 and electrodes. This demonstration of contact interface engineering with CVD‐grown MoS2 and graphene is a key step toward the practical application of atomically thin TMDC‐based devices

Published in: "Advanced Materials".

Ultrasensitive 2D Bi2O2Se Phototransistors on Silicon Substrates

2018-11-18T00:34:04+00:00November 17th, 2018|Categories: Publications|

Ultrasensitive Bi2O2Se phototransistors are demonstrated by utilizing a unique method to transfer CVD‐grown Bi2O2Se from mica onto silicon substrates. Compared with devices on mica, photodetectors on silicon maintain high photoresponsivity, high photoconductive gain, fast response rate, and at the same time, the dark current is much lowered, which yields ultrahigh on/off ratio and specific detectivity. Abstract 2D materials are considered as intriguing building blocks for next‐generation optoelectronic devices. However, their photoresponse performance still needs to be improved for practical applications. Here, ultrasensitive 2D phototransistors are reported employing chemical vapor deposition (CVD)‐grown 2D Bi2O2Se transferred onto silicon substrates with a noncorrosive transfer method. The as‐transferred Bi2O2Se preserves high quality in contrast to the serious quality degradation in hydrofluoric‐acid‐assisted transfer. The phototransistors show a responsivity of 3.5 × 104 A W−1, a photoconductive gain of more than 104, and a time response in the order of sub‐millisecond. With back gating of the silicon substrate, the dark current can be reduced to several pA. This yields an ultrahigh sensitivity with a specific detectivity of 9.0 × 1013 Jones, which is one of the highest values among 2D material photodetectors and two orders of magnitude higher than that of other CVD‐grown 2D materials. The high performance of the phototransistor shown here together with the developed unique transfer technique are promising for the development of novel 2D‐material‐based optoelectronic applications as well as integrating with state‐of‐the‐art silicon photonic and electronic technologies.

Published in: "Advanced Materials".

Direct CVD Growth of Graphene on Traditional Glass: Methods and Mechanisms

2018-11-18T00:34:01+00:00November 17th, 2018|Categories: Publications|Tags: |

A summary of the chemical vapor deposition (CVD) growth techniques of graphene on traditional glass as well as the growth mechanisms is provided. Direct thermal CVD growth, molten‐bed CVD growth, metal‐catalyst‐assisted growth, and plasma‐enhanced growth are covered. Emphasis is laid on the strategy of growth corresponding to the different natures of glass substrates. Abstract Chemical vapor deposition (CVD) on catalytic metal surfaces is considered to be the most effective way to obtain large‐area, high‐quality graphene films. For practical applications, a transfer process from metal catalysts to target substrates (e.g., poly(ethylene terephthalate) (PET), glass, and SiO2/Si) is unavoidable and severely degrades the quality of graphene. In particular, the direct growth of graphene on glass can avoid the tedious transfer process and endow traditional glass with prominent electrical and thermal conductivities. Such a combination of graphene and glass creates a new type of glass, the so‐called “super graphene glass,” which has attracted great interest from the viewpoints of both fundamental research and daily‐life applications. In the last few years, great progress has been achieved in pursuit of this goal. Here, these growth methods as well as the specific growth mechanisms of graphene on glass surfaces are summarized. The typical techniques developed include direct thermal CVD growth, molten‐bed CVD growth, metal‐catalyst‐assisted growth, and plasma‐enhanced growth. Emphasis is placed on the strategy of growth corresponding to the different natures of glass substrates. A comprehensive understanding of graphene growth on nonmetal glass substrates and the latest status of “super graphene glass” production are provided.

Published in: "Advanced Materials".

Rollable, Stretchable, and Reconfigurable Graphene Hygroelectric Generators

2018-11-18T00:33:59+00:00November 17th, 2018|Categories: Publications|Tags: |

Rollable, stretchable, and 3D space‐deformable graphene‐based hygroelectric generators are developed by a laser processing strategy, which exhibit excellent electricity‐generation ability without any significant performance loss despite being deformed arbitrarily, and are promising as power supply for applications in complicated conditions. Abstract Moisture‐triggered electricity generation has attracted much attention because of the effective utilization of the water‐molecule diffusion process widely existing in atmosphere. However, the monotonous and rigid structures of previously developed generators have heavily restricted their applications in complex and highly deformable working conditions. Herein, by a rational configuration design with a versatile laser processing strategy, graphene‐based hygroelectric generators (GHEGs) of sophisticated architectures with diversified functions such as rollable, stretchable, and even multidimensional transformation are achieved for the first time. More importantly, a wide range of 3D deformable generators that can automatically assemble and transform from planar geometries into spacial architectures are also successfully fabricated, including cubic boxes, pyramids, Miura‐ori, and footballs. These GHEGs demonstrate excellent electricity‐generation performance in curling and elongating states. The generated voltages are easily up to 1.5 V under humidity variation in atmosphere, powering a variety of commercial electronic components. These deformable GHEGs can be applied on complicated surfaces, human bodies, and many more beyond those demonstrated in this work.

Published in: "Advanced Materials".

Surface Effect on 2D Hybrid Perovskite Crystals: Perovskites Using an Ethanolamine Organic Layer as an Example

2018-11-18T00:33:58+00:00November 17th, 2018|Categories: Publications|

The influence of the surface effect of 2D layered perovskites before and after mechanical exfoliation is studied. The smooth 2D perovskite is less sensitive to ambient moisture and exhibits a considerably low dark current. This work reveals the strong dependence of the surface condition of 2D hybrid perovskite crystals on their moisture stability and optoelectronic properties. Abstract Despite the remarkable progress of optoelectronic devices based on hybrid perovskites, there are significant drawbacks, which have largely hindered their development as an alternative of silicon. For instance, hybrid perovskites are well‐known to suffer from moisture instability which leads to surface degradation. Nonetheless, the dependence of the surface effect on the moisture stability and optoelectronic properties of hybrid perovskites has not been fully investigated. In this work, the influence of the surface effect of 2D layered perovskites before and after mechanical exfoliation, representing rough and smooth surfaces of perovskite crystals, are studied. It is found that the smooth 2D perovskite is less sensitive to ambient moisture and exhibits a considerably low dark current, which outperforms the rough perovskites by 23.6 times in terms of photodetectivity. The superior moisture stability of the smooth perovskites over the rough perovskites is demonstrated. Additionally, ethanolamine is employed as an organic linker of the 2D layered perovskite, which further improves the moisture stability. This work reveals the strong dependence of the surface conditions of 2D hybrid perovskite crystals on their moisture stability and optoelectronic properties, which are of utmost importance to the design of practical optoelectronic devices

Published in: "Advanced Materials".

Stimuli‐Responsive Materials: Self‐Adapting Wettability of ReS2 under a Constant Stimulus (Adv. Mater. 46/2018)

2018-11-18T00:33:56+00:00November 17th, 2018|Categories: Publications|Tags: |

In article number 1804559, Lei Fu and co‐workers enforce a smart self‐adapting wettability (SAQ) of ReS2 under sustained light irradiation, which breaks the stereotype that a single stimulus leads to a monotonic change in properties or structure. This unique SAW provides a brand‐new insight to broaden the applications of responsive materials, which will undoubtedly pave a novel way in further device optimization.

Published in: "Advanced Materials".

2D Layered Perovskites: Surface Effect on 2D Hybrid Perovskite Crystals: Perovskites Using an Ethanolamine Organic Layer as an Example (Adv. Mater. 46/2018)

2018-11-18T00:33:53+00:00November 17th, 2018|Categories: Publications|

In article number 1804372, Jr‐Hau He and co‐workers study the influences of the surface effect of 2D layered perovskites before and after mechanical exfoliation. The smooth 2D perovskite is less sensitive to ambient moisture and exhibits a considerably low dark current. This work reveals the strong dependence of the surface condition of 2D hybrid perovskite crystals on their moisture stability and optoelectronic properties.

Published in: "Advanced Materials".

Direct CVD Growth of Graphene on Traditional Glass: Methods and Mechanisms

2018-11-17T02:35:38+00:00November 17th, 2018|Categories: Publications|Tags: |

A summary of the chemical vapor deposition (CVD) growth techniques of graphene on traditional glass as well as the growth mechanisms is provided. Direct thermal CVD growth, molten‐bed CVD growth, metal‐catalyst‐assisted growth, and plasma‐enhanced growth are covered. Emphasis is laid on the strategy of growth corresponding to the different natures of glass substrates. Abstract Chemical vapor deposition (CVD) on catalytic metal surfaces is considered to be the most effective way to obtain large‐area, high‐quality graphene films. For practical applications, a transfer process from metal catalysts to target substrates (e.g., poly(ethylene terephthalate) (PET), glass, and SiO2/Si) is unavoidable and severely degrades the quality of graphene. In particular, the direct growth of graphene on glass can avoid the tedious transfer process and endow traditional glass with prominent electrical and thermal conductivities. Such a combination of graphene and glass creates a new type of glass, the so‐called “super graphene glass,” which has attracted great interest from the viewpoints of both fundamental research and daily‐life applications. In the last few years, great progress has been achieved in pursuit of this goal. Here, these growth methods as well as the specific growth mechanisms of graphene on glass surfaces are summarized. The typical techniques developed include direct thermal CVD growth, molten‐bed CVD growth, metal‐catalyst‐assisted growth, and plasma‐enhanced growth. Emphasis is placed on the strategy of growth corresponding to the different natures of glass substrates. A comprehensive understanding of graphene growth on nonmetal glass substrates and the latest status of “super graphene glass” production are provided.

Published in: "Advanced Materials".

Rollable, Stretchable, and Reconfigurable Graphene Hygroelectric Generators

2018-11-17T02:35:36+00:00November 17th, 2018|Categories: Publications|Tags: |

Rollable, stretchable, and 3D space‐deformable graphene‐based hygroelectric generators are developed by a laser processing strategy, which exhibit excellent electricity‐generation ability without any significant performance loss despite being deformed arbitrarily, and are promising as power supply for applications in complicated conditions. Abstract Moisture‐triggered electricity generation has attracted much attention because of the effective utilization of the water‐molecule diffusion process widely existing in atmosphere. However, the monotonous and rigid structures of previously developed generators have heavily restricted their applications in complex and highly deformable working conditions. Herein, by a rational configuration design with a versatile laser processing strategy, graphene‐based hygroelectric generators (GHEGs) of sophisticated architectures with diversified functions such as rollable, stretchable, and even multidimensional transformation are achieved for the first time. More importantly, a wide range of 3D deformable generators that can automatically assemble and transform from planar geometries into spacial architectures are also successfully fabricated, including cubic boxes, pyramids, Miura‐ori, and footballs. These GHEGs demonstrate excellent electricity‐generation performance in curling and elongating states. The generated voltages are easily up to 1.5 V under humidity variation in atmosphere, powering a variety of commercial electronic components. These deformable GHEGs can be applied on complicated surfaces, human bodies, and many more beyond those demonstrated in this work.

Published in: "Advanced Materials".

Stimuli‐Responsive Materials: Self‐Adapting Wettability of ReS2 under a Constant Stimulus (Adv. Mater. 46/2018)

2018-11-13T10:35:59+00:00November 13th, 2018|Categories: Publications|Tags: |

In article number 1804559, Lei Fu and co‐workers enforce a smart self‐adapting wettability (SAQ) of ReS2 under sustained light irradiation, which breaks the stereotype that a single stimulus leads to a monotonic change in properties or structure. This unique SAW provides a brand‐new insight to broaden the applications of responsive materials, which will undoubtedly pave a novel way in further device optimization.

Published in: "Advanced Materials".

Surface Effect on 2D Hybrid Perovskite Crystals: Perovskites Using an Ethanolamine Organic Layer as an Example

2018-11-13T10:35:51+00:00November 13th, 2018|Categories: Publications|

The influence of the surface effect of 2D layered perovskites before and after mechanical exfoliation is studied. The smooth 2D perovskite is less sensitive to ambient moisture and exhibits a considerably low dark current. This work reveals the strong dependence of the surface condition of 2D hybrid perovskite crystals on their moisture stability and optoelectronic properties. Abstract Despite the remarkable progress of optoelectronic devices based on hybrid perovskites, there are significant drawbacks, which have largely hindered their development as an alternative of silicon. For instance, hybrid perovskites are well‐known to suffer from moisture instability which leads to surface degradation. Nonetheless, the dependence of the surface effect on the moisture stability and optoelectronic properties of hybrid perovskites has not been fully investigated. In this work, the influence of the surface effect of 2D layered perovskites before and after mechanical exfoliation, representing rough and smooth surfaces of perovskite crystals, are studied. It is found that the smooth 2D perovskite is less sensitive to ambient moisture and exhibits a considerably low dark current, which outperforms the rough perovskites by 23.6 times in terms of photodetectivity. The superior moisture stability of the smooth perovskites over the rough perovskites is demonstrated. Additionally, ethanolamine is employed as an organic linker of the 2D layered perovskite, which further improves the moisture stability. This work reveals the strong dependence of the surface conditions of 2D hybrid perovskite crystals on their moisture stability and optoelectronic properties, which are of utmost importance to the design of practical optoelectronic devices

Published in: "Advanced Materials".

2D Layered Perovskites: Surface Effect on 2D Hybrid Perovskite Crystals: Perovskites Using an Ethanolamine Organic Layer as an Example (Adv. Mater. 46/2018)

2018-11-13T10:35:49+00:00November 13th, 2018|Categories: Publications|

In article number 1804372, Jr‐Hau He and co‐workers study the influences of the surface effect of 2D layered perovskites before and after mechanical exfoliation. The smooth 2D perovskite is less sensitive to ambient moisture and exhibits a considerably low dark current. This work reveals the strong dependence of the surface condition of 2D hybrid perovskite crystals on their moisture stability and optoelectronic properties.

Published in: "Advanced Materials".

Ultrasensitive 2D Bi2O2Se Phototransistors on Silicon Substrates

2018-11-13T10:35:47+00:00November 13th, 2018|Categories: Publications|

Ultrasensitive Bi2O2Se phototransistors are demonstrated by utilizing a unique method to transfer CVD‐grown Bi2O2Se from mica onto silicon substrates. Compared with devices on mica, photodetectors on silicon maintain high photoresponsivity, high photoconductive gain, fast response rate, and at the same time, the dark current is much lowered, which yields ultrahigh on/off ratio and specific detectivity. Abstract 2D materials are considered as intriguing building blocks for next‐generation optoelectronic devices. However, their photoresponse performance still needs to be improved for practical applications. Here, ultrasensitive 2D phototransistors are reported employing chemical vapor deposition (CVD)‐grown 2D Bi2O2Se transferred onto silicon substrates with a noncorrosive transfer method. The as‐transferred Bi2O2Se preserves high quality in contrast to the serious quality degradation in hydrofluoric‐acid‐assisted transfer. The phototransistors show a responsivity of 3.5 × 104 A W−1, a photoconductive gain of more than 104, and a time response in the order of sub‐millisecond. With back gating of the silicon substrate, the dark current can be reduced to several pA. This yields an ultrahigh sensitivity with a specific detectivity of 9.0 × 1013 Jones, which is one of the highest values among 2D material photodetectors and two orders of magnitude higher than that of other CVD‐grown 2D materials. The high performance of the phototransistor shown here together with the developed unique transfer technique are promising for the development of novel 2D‐material‐based optoelectronic applications as well as integrating with state‐of‐the‐art silicon photonic and electronic technologies.

Published in: "Advanced Materials".

Cellular Networks: A Plesiohedral Cellular Network of Graphene Bubbles for Ultralight, Strong, and Superelastic Materials (Adv. Mater. 45/2018)

2018-11-10T22:35:18+00:00November 10th, 2018|Categories: Publications|Tags: |

The design and synthesis of lightweight and strong materials are essential for developing next‐generation structural materials. In article number 1802997, Seok Joon Kwon, Pil J. Yoo, and co‐workers demonstrate a new class of graphene‐based, ultralight, strong, and superelastic closed‐cellular structures by developing an innovative hierarchical architecturing strategy. The achieved structure is a uniformly ordered plesiohedral cellular structure with complete space‐filling convex polytopes.

Published in: "Advanced Materials".

Organic‐Single‐Crystal Vertical Field‐Effect Transistors and Phototransistors

2018-11-10T22:35:12+00:00November 10th, 2018|Categories: Publications|Tags: |

Organic‐single‐crystal vertical field‐effect transistors and phototransistors based on the 2,6‐diphenyl anthracene compound are fabricated, which exhibit a high on/off ratio up to 106, and superior photoresponse performance with photoresponsivity of 110 A W−1 and detectivity of 1013 Jones under light illumination, which indicates their great potential in integrated optoelectronic devices. Abstract Organic vertical field‐effect transistors (VFETs) have attracted significant attention over the past years due to their unique characteristics of high output currents, low operation voltages, high working frequency, and promising high‐density integration for circuits. However, most currently reported VFETs demonstrate poor performance, e.g., with low on/off ratio and current density. Here, the first organic‐single‐crystal vertical field‐effect transistors (SC‐VFETs) and phototransistors are constructed from 2,6‐diphenyl anthracene (DPA) through a modified method. The devices exhibit high on/off ratio of 106 and a high current density of 100 mA cm‐2 under a small voltage of −5 V, which are proved to be one of the best performances for organic VFETs. Furthermore, superior photoresponse performance with photoresponsivity of 110 A W‐1 and detectivity of 1013 Jones is obtained under light illumination for vertical phototransistors. These results confirm the control of the intrinsic Schottky barrier height at the graphene–DPA junction along with good interfacial contact effectively suppressing the dark current to realize a large on/off ratio and high light detectivity. This vertical integration of graphene with organic single crystals via simple, effective fabrication processes opens up new opportunities to realize high‐performance integrated organic vertical electronic and optoelectronic devices.

Published in: "Advanced Materials".

Hydrogen Evolution Reaction: Mechanochemically Assisted Synthesis of a Ru Catalyst for Hydrogen Evolution with Performance Superior to Pt in Both Acidic and Alkaline Media (Adv. Mater. 44/2018)

2018-11-10T22:35:10+00:00November 10th, 2018|Categories: Publications|Tags: |

In article number 1803676, In‐Yup Jeon, Jong‐Beom Baek, and co‐workers develop a method for low‐cost and scalable production of a ruthenium (Ru) on graphene nanoplatelet (GnP) catalyst for the hydrogen evolution reaction (HER) via a mechanochemically assisted approach. The [email protected] catalyst exhibits HER performance superior to commercial Pt/C in both acidic and alkaline media. The simple mechanochemical approach offers large‐scale production for commercial applications.

Published in: "Advanced Materials".

Promoted Glycerol Oxidation Reaction in an Interface‐Confined Hierarchically Structured Catalyst

2018-11-10T22:35:06+00:00November 10th, 2018|Categories: Publications|Tags: , |

The confinement of Pt nanosheets is realized in a vertically erected graphene array with hierarchically porous architecture to address the mass‐diffusion limitation in interface‐confined catalysis. Such a confined 3D catalyst exhibits a much stronger oxidation and CC bond cleaving ability for the glycerol oxidation reaction, leading to a superior mass activity and selectivity toward C1 products than commercial Pt/C catalysts. Abstract Confined catalysis in a 2D system is of particular interest owing to the facet control of the catalysts and the anisotropic kinetics of reactants, which suppress side reactions and improve selectivity. Here, a 2D‐confined system consisting of intercalated Pt nanosheets within few‐layered graphene is demonstrated. The strong metal–substrate interaction between the Pt nanosheets and the graphene leads to the quasi‐2D growth of Pt with a unique (100)/(111)/(100) faceted structure, thus providing excellent catalytic activity and selectivity toward one‐carbon (C1) products for the glycerol oxidation reaction. A hierarchically porous graphene architecture, grown on carbon cloth, is used to fabricate the confined catalyst bed in order to enhance the mass‐diffusion limitation in interface‐confined reactions. Owing to its unique 3D porous structure, this graphene‐confined Pt catalyst exhibits an extraordinary mass activity of 2910 mA mgPt−1 together with a formate selectivity of 79% at 60 °C. This paves the way toward rational designs of heterogeneous catalysts for energy‐related applications.

Published in: "Advanced Materials".

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