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Journal ArticleDOI: 10.1039/D0CC08261A

Electrochemically captured Zintl cluster-induced bismuthene for sodium-ion storage.

04 Mar 2021-Chemical Communications (Royal Society of Chemistry (RSC))-Vol. 57, Iss: 19, pp 2396-2399
Abstract: Bismuthene was prepared via the oxidation of Zintl clusters by electrochemical cathodic corrosion. It was found that the conversion of Zintl clusters from Bi22- to Bi2 occurred in the electrolyte having short alkyl chains due to the faster kinetics of highly reactive carbocation. Considering that c-Na3Bi exists in a wide voltage range, monitored by in situ XRD, a new wide peak for the as-obtained bismuthene in the CV curve was noticed, which benefits the improvement of electrochemical performances.

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Topics: Electrochemistry (50%)

5 results found

Journal ArticleDOI: 10.1021/ACSNANO.1C00304
Jun Chen1, Wentao Deng1, Xu Gao1, Shouyi Yin1  +5 moreInstitutions (1)
01 Apr 2021-ACS Nano
Abstract: The practical application of lithium-ion batteries suffers from low energy density and the struggle to satisfy the ever-growing requirements of the energy-storage Internet Therefore, developing next-generation electrode materials with high energy density is of the utmost significance There are high expectations with respect to the development of lattice oxygen redox (LOR)-a promising strategy for developing cathode materials as it renders nearly a doubling of the specific capacity However, challenges have been put forward toward the deep-seated origins of the LOR reaction and if its whole potential could be effectively realized in practical application In the following Review, the intrinsic science that induces the LOR activity and crystal structure evolution are extensively discussed Moreover, a variety of characterization techniques for investigating these behaviors are presented Furthermore, we have highlighted the practical restrictions and outlined the probable approaches of Li-based layered oxide cathodes for improving such materials to meet the practical applications

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8 Citations

Journal ArticleDOI: 10.1016/J.ENSM.2021.10.019
Anni Wang1, Wanwan Hong1, Lin Li1, Ruiting Guo1  +6 moreInstitutions (2)
Abstract: Graphical abstract CDs are utilized as crucial structure-directing agents to elaborately design 3D cross-linked rod-like structured Bi2Se3/CDs composites. Computational simulations combined with experiments demonstrate that such robust 3D framework and the existence of interface Bi-O-C bond can simultaneously enhance the intrinsic sluggish kinetics and structural stability, endowing Bi2Se3/CDs anode with fast-charging capability and durable cycling life. Download : Download high-res image (205KB) Download : Download full-size image Advanced electrode materials for fast-charging lithium-ion batteries are of great significance to next-generation energy-storage systems. Herein, three-dimensional (3D) hierarchical rod-structured Bi2Se3/carbon dots (Bi2Se3/CDs) composite is elaborately designed for fast-kinetics lithium storage. It is proposed that CDs-induced self-assembly growth and site-selective ion-exchange transform nanosheets into cross-linked architecture. Such robust 3D framework provides efficient channels for electron/ion transport and sufficient inner space for volume variation as confirmed by theoretical prediction. Notably, the existence of interface Bi-O-C bond would effectively enhance its inherent bulk electronic conductivity and accelerate ionic transportation by narrowing the bandgap and reducing the Li+ migration energy barriers. Consequently, intrinsic sluggish kinetics and structural stability are simultaneously improved, endowing Bi2Se3/CDs composite electrode fast charging/discharging capability of 165 mAh g−1 at 20 A g−1 (corresponding to charge in ≈27 s) and excellent long-term durability with the capacity of 502 mAh g−1 over 950 cycles at 1 A g−1. Moreover, the intercalation-conversion-alloying type lithium storage mechanism of Bi2Se3/CDs is revealed by in-situ XRD. This work provides a train of thoughts for other CDs-tailored composites with tunable morphology and structure.

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1 Citations

Open accessJournal ArticleDOI: 10.1016/J.JECHEM.2021.10.038
Laiqiang Xu1, Jiayang Li1, Honglei Shuai1, Zheng Luo1  +6 moreInstitutions (1)
Abstract: All-solid-state lithium batteries (ASSLBs) are recognized as high energy density batteries system without safety issues within the next generation of batteries. The development of solid electrolytes is the crucial step of ASSLBs. The composite electrolyte has stable physical and electrochemical characteristics, and its comprehensive performance surpasses the individual solid electrolyte, bringing unique vitality to the solid electrolyte. However, their intrinsic weakness limits the development of composite electrolytes. In this review, we provide a comprehensive and in-depth understanding of the challenges and opportunities of composite electrolytes, with special focus on mechanisms of ion transport, nanostructure design towards high ionic conductivity, interfacial issues within electrolytes and electrodes. Furthermore, future development is prospected, which can shed light on researchers in this field and accelerate the industrial production of composite electrolytes.

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Topics: Fast ion conductor (55%)

Journal ArticleDOI: 10.1002/ADFM.202107280
Abstract: Graphene and related elemental 2D materials have become core materials in nanotechnology and shown great promise for industrially important electrocatalysis reactions. Although excellent progress has been made over the past few years, research into the field of elemental 2D materials beyond graphene is still at an early stage. Importantly, recent research has revealed the promising efficacy of elemental 2D materials as effective nitrogen reduction reaction (NRR) electrocatalysts due to their many excellent properties including high surface activities, acting as active sites for effective functionalization and defect engineering. This review provides a comprehensive account of recent advances in elemental 2D materials with a major focus on the solution-based synthesis routes and their applications in electrocatalytic NRR for ammonia (NH3) production. After a concise overview of elemental 2D materials, the advantages and challenges of currently available methods for the synthesis of these 2D materials are discussed. Then, the review focuses on the use of these emerging 2D materials in the electrocatalytic reduction of N2 for sustainable (NH3) synthesis. Finally, the challenges still to be addressed, and important perspectives in this attractive field are emphasized.

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Open accessJournal ArticleDOI: 10.1016/J.CEJ.2021.133841
Susu Fang1, Jiayang Li1, Kangyu Zou1, Honglei Shuai1  +5 moreInstitutions (1)
Abstract: Since the discovery of Zintl phases in the 1891s, they have attracted considerable interests because of their novel structures, fascinated bonding and special physical properties. However, the research about Zintl phases is not complete, limiting the development of this discipline. Hence, in this work we systematically introduce the preparation approaches of Zintl phases and Zintl anions to understand the originations of their attractive structures. More importantly, the recent developments about their applications (such as thermoelectricity, catalysis, superconductor and magnetism) are thoroughly concluded. Especially, their devotions utilized as precursors for preparing functional materials are summarized. Additionally, the remaining challenges and perspectives of Zintl phases are further discussed. This review is aimed to provide a comprehensive understanding of the Zintl phases, offering a directional guideline towards broad applications.

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20 results found

Journal ArticleDOI: 10.1038/NATURE08308
Pedram Roushan1, Jungpil Seo, Colin V. Parker, Yew San Hor1  +6 moreInstitutions (1)
27 Aug 2009-Nature
Abstract: Topological insulators are a new class of insulators in which a bulk gap for electronic excitations is generated because of the strong spin–orbit coupling inherent to these systems. These materials are distinguished from ordinary insulators by the presence of gapless metallic surface states, resembling chiral edge modes in quantum Hall systems, but with unconventional spin textures. A key predicted feature of such spin-textured boundary states is their insensitivity to spin-independent scattering, which is thought to protect them from backscattering and localization. Recently, experimental and theoretical efforts have provided strong evidence for the existence of both two- and three-dimensional classes of such topological insulator materials in semiconductor quantum well structures and several bismuth-based compounds, but so far experiments have not probed the sensitivity of these chiral states to scattering. Here we use scanning tunnelling spectroscopy and angle-resolved photoemission spectroscopy to visualize the gapless surface states in the three-dimensional topological insulator Bi_(1-x)Sb_x, and examine in detail the influence of scattering from disorder caused by random alloying in this compound. We show that, despite strong atomic scale disorder, backscattering between states of opposite momentum and opposite spin is absent. Our observations demonstrate that the chiral nature of these states protects the spin of the carriers. These chiral states are therefore potentially useful for spin-based electronics, in which long spin coherence is critical, and also for quantum computing applications, where topological protection can enable fault-tolerant information processing.

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Topics: Topological insulator (68%), Topological order (65%), Spin states (56%) ... read more

779 Citations

Journal ArticleDOI: 10.1002/ANIE.201507568
Shengli Zhang1, Meiqiu Xie1, Fengyu Li2, Zhong Yan1  +5 moreInstitutions (3)
26 Jan 2016-Angewandte Chemie
Abstract: Optoelectronic applications require materials both responsive to objective photons and able to transfer carriers, so new two-dimensional (2D) semiconductors with appropriate band gaps and high mobilities are highly desired. A broad range of band gaps and high mobilities of a 2D semiconductor family, composed of monolayer of Group 15 elements (phosphorene, arsenene, antimonene, bismuthene) is presented. The calculated binding energies and phonon band dispersions of 2D Group 15 allotropes exhibit thermodynamic stability. The energy band gaps of 2D semiconducting Group 15 monolayers cover a wide range from 0.36 to 2.62 eV, which are crucial for broadband photoresponse. Significantly, phosphorene, arsenene, and bismuthene possess carrier mobilities as high as several thousand cm2 V−1 s−1. Combining such broad band gaps and superior carrier mobilities, 2D Group 15 monolayers are promising candidates for nanoelectronics and optoelectronics.

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Topics: Band gap (59%), Phosphorene (59%), Electronic band structure (51%)

631 Citations

Open accessJournal ArticleDOI: 10.1103/PHYSREVLETT.93.105501
T. Nagao1, T. Nagao2, Jerzy T. Sadowski1, M. Saito3  +7 moreInstitutions (4)
Abstract: Our scanning tunneling microscopy and electron diffraction experiments revealed that a new two-dimensional allotrope of Bi forms on the Si(111)-7x7 surface. This pseudocubic [012]-oriented allotrope is stable up to four atomic layers at room temperature. Above this critical thickness, the entire volume of the film starts to transform into a bulk single-crystal (001) phase, as the bulk contribution in the cohesion becomes dominant. Based on ab initio calculations, we propose that the new allotrope consists of black phosphorus-like puckered layers stabilized by saturating all the p(z) dangling bonds in the film.

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315 Citations

Journal ArticleDOI: 10.1021/ACSCATAL.9B00366
Laiquan Li1, Cheng Tang1, Bingquan Xia1, Huanyu Jin1  +2 moreInstitutions (1)
21 Feb 2019-ACS Catalysis
Abstract: Electrochemical fixation of N2 to ammonia is a promising strategy to store renewable energy and mitigate greenhouse gas emissions. However, it usually suffers from extremely low ammonia yield and Faradaic efficiency because of the lack of efficient electrocatalysts and the competing hydrogen evolution reaction. Herein, we report that the semiconducting bismuth can be a promising catalyst for ambient electrocatalytic N2 reduction reaction (NRR). A two-dimensional mosaic bismuth nanosheet (Bi NS) was fabricated via an in situ electrochemical reduction process and exhibited favorable average ammonia yield and Faradaic efficiency as high as 2.54 ± 0.16 μgNH3 cm–2 h–1 (∼13.23 μg mgcat.–1 h–1) and 10.46 ± 1.45% at −0.8 V versus reversible hydrogen electrode in 0.1 M Na2SO4. The high NRR electrocatalytic activity of the Bi NS could be attributed to the sufficient exposure of edge sites coupled with effective p-orbital electron delocalization in the mosaic bismuth nanosheets. In addition, the semiconducting featu...

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Topics: Bismuth (55%), Reversible hydrogen electrode (54%), Electrocatalyst (54%)

273 Citations

Open accessJournal ArticleDOI: 10.1038/S41467-020-14914-9
Yang Fa1, Yang Fa2, Ahmed O. Elnabawy3, Roberto Schimmenti3  +10 moreInstitutions (3)
Abstract: Bismuth (Bi) has been known as a highly efficient electrocatalyst for CO2 reduction reaction. Stable free-standing two-dimensional Bi monolayer (Bismuthene) structures have been predicted theoretically, but never realized experimentally. Here, we show the first simple large-scale synthesis of free-standing Bismuthene, to our knowledge, and demonstrate its high electrocatalytic efficiency for formate (HCOO−) formation from CO2 reduction reaction. The catalytic performance is evident by the high Faradaic efficiency (99% at −580 mV vs. Reversible Hydrogen Electrode (RHE)), small onset overpotential (<90 mV) and high durability (no performance decay after 75 h and annealing at 400 °C). Density functional theory calculations show the structure-sensitivity of the CO2 reduction reaction over Bismuthene and thicker nanosheets, suggesting that selective formation of HCOO− indeed can proceed easily on Bismuthene (111) facet due to the unique compressive strain. This work paves the way for the extensive experimental investigation of Bismuthene in many different fields. Stable free-standing two-dimensional Bi monolayer (Bismuthene) structures have been predicted theoretically, but never realized experimentally. Here, the authors show a large-scale synthesis of free-standing Bismuthene and its electrocatalytic activity for CO2 reduction to formate.

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Topics: Overpotential (54%), Electrocatalyst (53%), Reversible hydrogen electrode (52%) ... read more

95 Citations