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Wenhua Zhang

Bio: Wenhua Zhang is an academic researcher from University of Science and Technology of China. The author has contributed to research in topics: Catalysis & Medicine. The author has an hindex of 47, co-authored 190 publications receiving 9255 citations. Previous affiliations of Wenhua Zhang include Australian National University & Huazhong University of Science and Technology.


Papers
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Journal ArticleDOI
07 Jan 2016-Nature
TL;DR: In this paper, the role of the two different catalytic sites of pure cobalt and coexisting domains of cobalt metal and cobalt oxide has been evaluated, showing that surface cobalt atoms of the atomically thin layers have higher intrinsic activity and selectivity towards formate production, at lower overpotentials.
Abstract: Electroreduction of CO2 into useful fuels, especially if driven by renewable energy, represents a potentially 'clean' strategy for replacing fossil feedstocks and dealing with increasing CO2 emissions and their adverse effects on climate. The critical bottleneck lies in activating CO2 into the CO2(•-) radical anion or other intermediates that can be converted further, as the activation usually requires impractically high overpotentials. Recently, electrocatalysts based on oxide-derived metal nanostructures have been shown to enable CO2 reduction at low overpotentials. However, it remains unclear how the electrocatalytic activity of these metals is influenced by their native oxides, mainly because microstructural features such as interfaces and defects influence CO2 reduction activity yet are difficult to control. To evaluate the role of the two different catalytic sites, here we fabricate two kinds of four-atom-thick layers: pure cobalt metal, and co-existing domains of cobalt metal and cobalt oxide. Cobalt mainly produces formate (HCOO(-)) during CO2 electroreduction; we find that surface cobalt atoms of the atomically thin layers have higher intrinsic activity and selectivity towards formate production, at lower overpotentials, than do surface cobalt atoms on bulk samples. Partial oxidation of the atomic layers further increases their intrinsic activity, allowing us to realize stable current densities of about 10 milliamperes per square centimetre over 40 hours, with approximately 90 per cent formate selectivity at an overpotential of only 0.24 volts, which outperforms previously reported metal or metal oxide electrodes evaluated under comparable conditions. The correct morphology and oxidation state can thus transform a material from one considered nearly non-catalytic for the CO2 electroreduction reaction into an active catalyst. These findings point to new opportunities for manipulating and improving the CO2 electroreduction properties of metal systems, especially once the influence of both the atomic-scale structure and the presence of oxide are mechanistically better understood.

1,407 citations

Journal ArticleDOI
TL;DR: Pt2 dimers can be fabricated with a bottom–up approach on graphene using atomic layer deposition, through proper nucleation sites creation, Pt1 single-atom deposition and attaching a secondary Pt atom selectively on the preliminary one.
Abstract: Supported metal clusters containing only a few atoms are of great interest. Progress has been made in synthesis of metal single-atom catalysts. However, precise synthesis of metal dimers on high-surface area support remains a grand challenge. Here, we show that Pt2 dimers can be fabricated with a bottom–up approach on graphene using atomic layer deposition, through proper nucleation sites creation, Pt1 single-atom deposition and attaching a secondary Pt atom selectively on the preliminary one. Scanning transmission electron microscopy, x-ray absorption spectroscopy, and theoretical calculations suggest that the Pt2 dimers are likely in the oxidized form of Pt2Ox. In hydrolytic dehydrogenation of ammonia borane, Pt2 dimers exhibit a high specific rate of 2800 molH2 molPt −1 min−1 at room temperature, ~17- and 45-fold higher than graphene supported Pt single atoms and nanoparticles, respectively. These findings open an avenue to bottom–up fabrication of supported atomically precise ultrafine metal clusters for practical applications. Controlled fabrication of few-atoms supported catalysts is a major challenge in the synthesis of nanomaterials. Here, the authors show a bottom-up approach to precisely synthesize platinum dimers supported on graphene, which display higher catalytic activity and stability than single atoms and nanoparticles.

645 citations

Journal ArticleDOI
TL;DR: It is demonstrated that the synergetic interaction between neighbouring Pt monomers on MoS2 greatly enhanced the CO2 hydrogenation catalytic activity and reduced the activation energy relative to isolated monomers.
Abstract: Exploring the interaction between two neighbouring monomers has great potential to significantly raise the performance and deepen the mechanistic understanding of heterogeneous catalysis. Herein, we demonstrate that the synergetic interaction between neighbouring Pt monomers on MoS2 greatly enhanced the CO2 hydrogenation catalytic activity and reduced the activation energy relative to isolated monomers. Neighbouring Pt monomers were achieved by increasing the Pt mass loading up to 7.5% while maintaining the atomic dispersion of Pt. Mechanistic studies reveal that neighbouring Pt monomers not only worked in synergy to vary the reaction barrier, but also underwent distinct reaction paths compared with isolated monomers. Isolated Pt monomers favour the conversion of CO2 into methanol without the formation of formic acid, whereas CO2 is hydrogenated stepwise into formic acid and methanol for neighbouring Pt monomers. The discovery of the synergetic interaction between neighbouring monomers may create a new path for manipulating catalytic properties.

503 citations

Journal ArticleDOI
TL;DR: Atomic layers for transition-metal oxides are proposed to address problems of conventional electrocatalysts through offering an ultralarge fraction of active sites, high electronic conductivity, and superior structural stability.
Abstract: Electroreduction of CO2 into hydrocarbons could contribute to alleviating energy crisis and global warming. However, conventional electrocatalysts usually suffer from low energetic efficiency and poor durability. Herein, atomic layers for transition-metal oxides are proposed to address these problems through offering an ultralarge fraction of active sites, high electronic conductivity, and superior structural stability. As a prototype, 1.72 and 3.51 nm thick Co3O4 layers were synthesized through a fast-heating strategy. The atomic thickness endowed Co3O4 with abundant active sites, ensuring a large CO2 adsorption amount. The increased and more dispersed charge density near Fermi level allowed for enhanced electronic conductivity. The 1.72 nm thick Co3O4 layers showed over 1.5 and 20 times higher electrocatalytic activity than 3.51 nm thick Co3O4 layers and bulk counterpart, respectively. Also, 1.72 nm thick Co3O4 layers showed formate Faradaic efficiency of over 60% in 20 h.

398 citations

Journal ArticleDOI
29 Mar 2011-ACS Nano
TL;DR: A revised CVD route to grow graphene on Cu foils at low temperature, adopting solid and liquid hydrocarbon feedstocks, and the successful low-temperature growth can be qualitatively understood from the first principles calculations.
Abstract: Graphene has attracted a lot of research interest owing to its exotic properties and a wide spectrum of potential applications. Chemical vapor deposition (CVD) from gaseous hydrocarbon sources has shown great promises for large-scale graphene growth. However, high growth temperature, typically 1000 °C, is required for such growth. Here we demonstrate a revised CVD route to grow graphene on Cu foils at low temperature, adopting solid and liquid hydrocarbon feedstocks. For solid PMMA and polystyrene precursors, centimeter-scale monolayer graphene films are synthesized at a growth temperature down to 400 °C. When benzene is used as the hydrocarbon source, monolayer graphene flakes with excellent quality are achieved at a growth temperature as low as 300 °C. The successful low-temperature growth can be qualitatively understood from the first principles calculations. Our work might pave a way to an undemanding route for economical and convenient graphene growth.

392 citations


Cited by
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28 Jul 2005
TL;DR: PfPMP1)与感染红细胞、树突状组胞以及胎盘的单个或多个受体作用,在黏附及免疫逃避中起关键的作�ly.
Abstract: 抗原变异可使得多种致病微生物易于逃避宿主免疫应答。表达在感染红细胞表面的恶性疟原虫红细胞表面蛋白1(PfPMP1)与感染红细胞、内皮细胞、树突状细胞以及胎盘的单个或多个受体作用,在黏附及免疫逃避中起关键的作用。每个单倍体基因组var基因家族编码约60种成员,通过启动转录不同的var基因变异体为抗原变异提供了分子基础。

18,940 citations

Journal ArticleDOI
TL;DR: This review will be of value to synthetic chemists interested in this emerging field of materials science, as well as those investigating applications of graphene who would find a more thorough treatment of the chemistry of graphene oxide useful in understanding the scope and limitations of current approaches which utilize this material.
Abstract: The chemistry of graphene oxide is discussed in this critical review Particular emphasis is directed toward the synthesis of graphene oxide, as well as its structure Graphene oxide as a substrate for a variety of chemical transformations, including its reduction to graphene-like materials, is also discussed This review will be of value to synthetic chemists interested in this emerging field of materials science, as well as those investigating applications of graphene who would find a more thorough treatment of the chemistry of graphene oxide useful in understanding the scope and limitations of current approaches which utilize this material (91 references)

10,126 citations

Journal ArticleDOI
TL;DR: The unique advances on ultrathin 2D nanomaterials are introduced, followed by the description of their composition and crystal structures, and the assortments of their synthetic methods are summarized.
Abstract: Since the discovery of mechanically exfoliated graphene in 2004, research on ultrathin two-dimensional (2D) nanomaterials has grown exponentially in the fields of condensed matter physics, material science, chemistry, and nanotechnology. Highlighting their compelling physical, chemical, electronic, and optical properties, as well as their various potential applications, in this Review, we summarize the state-of-art progress on the ultrathin 2D nanomaterials with a particular emphasis on their recent advances. First, we introduce the unique advances on ultrathin 2D nanomaterials, followed by the description of their composition and crystal structures. The assortments of their synthetic methods are then summarized, including insights on their advantages and limitations, alongside some recommendations on suitable characterization techniques. We also discuss in detail the utilization of these ultrathin 2D nanomaterials for wide ranges of potential applications among the electronics/optoelectronics, electrocat...

3,628 citations

Journal ArticleDOI
TL;DR: Graphene has emerged as a subject of enormous scientific interest due to its exceptional electron transport, mechanical properties, and high surface area, and when incorporated appropriately, these atomically thin carbon sheets can significantly improve physical properties of host polymers at extremely small loading.
Abstract: Graphene has emerged as a subject of enormous scientific interest due to its exceptional electron transport, mechanical properties, and high surface area. When incorporated appropriately, these atomically thin carbon sheets can significantly improve physical properties of host polymers at extremely small loading. We first review production routes to exfoliated graphite with an emphasis on top-down strategies starting from graphite oxide, including advantages and disadvantages of each method. Then solvent- and melt-based strategies to disperse chemically or thermally reduced graphene oxide in polymers are discussed. Analytical techniques for characterizing particle dimensions, surface characteristics, and dispersion in matrix polymers are also introduced. We summarize electrical, thermal, mechanical, and gas barrier properties of the graphene/polymer nanocomposites. We conclude this review listing current challenges associated with processing and scalability of graphene composites and future perspectives f...

2,979 citations

Journal ArticleDOI
07 Jan 2011-Polymer
TL;DR: A survey of the literature on polymer nanocomposites with graphene-based fillers including recent work using graphite nanoplatelet fillers is presented in this article, along with methods for dispersing these materials in various polymer matrices.

2,782 citations