Search Results

You searched for all publications:

with publication states 'Published (Approved)'
published in journal 'Acs Energy Letters'

Search Again...

These results only include publications that have been reviewed and processed by Diamond Light Source. To also view papers that have not yet been processed click here.

You can use the folder icon under Actions to collate papers as required. You can then click on View Folder in the left-hand navigation to review and/or download your folder.

Exact matches
Related results

13 items found (0 items not approved), displaying 1 to 10.[First/Prev] 1, 2 [Next/Last]

Instruments / Technical Area	Publication Details	Published
	Operando measurement of layer breathing modes in lithiated graphite Hossein Yadegari , Mohamed A. Koronfel , Kang Wang , Daisy B. Thornton , Ifan E. L. Stephens , Carla Molteni , Peter D. Haynes , Mary P. Ryan Acs Energy Letters 220, 1633 - 1638 DOI: 10.1021/acsenergylett.1c00494 Show Abstract ▼ Abstract: Despite their ubiquitous usage and increasing societal dependence on Li-ion batteries, there remains a lack of detailed empirical evidence of Li intercalation/deintercalation into graphite even though this process dictates the performance, longevity, and safety of the system. Here, we report direct detection and dissociation of specific crystallographic phases in the lithiated graphite, which form through a stepwise staging process. Using operando measurements, LiC18, LiC12, and LiC6 phases are observed via distinct low-frequency Raman features, which are the result of displacement of the graphite lattice by induced local strain. Density functional theory calculations confirm the nature of the Raman-active vibrational modes, to the layer breathing modes (LBMs) of the lithiated graphite. The new findings indicate graphene-like characteristics in the lithiated graphite under the deep charged condition due to the imposed strain by the inserted Li. Moreover, our approach also provides a simple experimental tool to measure induced strain in the graphite structure under full intercalation conditions.	Apr 2021
	Rapid recombination by cadmium vacancies in CdTe Seán R. Kavanagh , Aron Walsh , David O. Scanlon Acs Energy Letters 6, 1392 - 1398 DOI: 10.1021/acsenergylett.1c00380 Open Access Show Abstract ▼ Abstract: CdTe is currently the largest thin-film photovoltaic technology. Non-radiative electron–hole recombination reduces the solar conversion efficiency from an ideal value of 32% to a current champion performance of 22%. The cadmium vacancy (VCd) is a prominent acceptor species in p-type CdTe; however, debate continues regarding its structural and electronic behavior. Using ab initio defect techniques, we calculate a negative-U double-acceptor level for VCd, while reproducing the VCd1– hole–polaron, reconciling theoretical predictions with experimental observations. We find the cadmium vacancy facilitates rapid charge-carrier recombination, reducing maximum power-conversion efficiency by over 5% for untreated CdTe—a consequence of tellurium dimerization, metastable structural arrangements, and anharmonic potential energy surfaces for carrier capture.	Mar 2021
	Operando generated ordered heterogeneous catalyst for the selective conversion of CO2 to methanol Arjun Cherevotan , Jithu Raj , Lakshay Dheer , Soumyabrata Roy , Shreya Sarkar , Risov Das , Chathakudath P. Vinod , Shaojun Xu , Peter Wells , Umesh V. Waghmare , Sebastian C. Peter Acs Energy Letters DOI: 10.1021/acsenergylett.0c02614 Show Abstract ▼ Abstract: The discovery of new materials for efficient transformation of carbon dioxide (CO2) into desired fuel can revolutionize large-scale renewable energy storage and mitigate environmental damage due to carbon emissions. In this work, we discovered an operando generated stable Ni–In kinetic phase that selectively converts CO2 to methanol (CTM) at low pressure compared to the state-of-the-art materials. The catalytic nature of a well-known methanation catalyst, nickel, has been tuned with the introduction of inactive indium, which enhances the CTM process. The remarkable change in the mechanistic pathways toward methanol production has been mapped by operando diffuse reflectance infrared Fourier transform spectroscopy analysis, corroborated by first-principles calculations. The ordered arrangement and pronounced electronegativity difference between metals are attributed to the complete shift in mechanism. The approach and findings of this work provide a unique advance toward the next-generation catalyst discovery for going beyond the state-of-the-art in CO2 reduction technologies.	Jan 2021
I11-High Resolution Powder Diffraction	In situ phase transformation on nickel-based selenides for enhanced hydrogen evolution reaction in alkaline medium Lingling Zhai , Tsz Woon Benedict Lo , Zheng-long Xu , Jonathan Potter , Jiaying Mo , Xuyun Guo , Chiu Chung Tang , Shik Chi Edman Tsang , Shu Ping Lau Acs Energy Letters DOI: 10.1021/acsenergylett.0c01385 Diamond Proposal Number(s): [23230] Show Abstract ▼ Abstract: Identification of the active species in electrocatalysts toward hydrogen evolution reaction (HER) is of great significance for the development of the catalytic industry; however, it is still the subject of considerable controversy. Herein, we applied operando synchrotron X-ray powder diffraction (SXRD) in the NiSe2 electrocatalyst system, and an in situ phase transformation from cubic NiSe2 to hexagonal NiSe was revealed. The NiSe phase showed an enhanced catalytic activity. Operando Raman spectroscopy verified the decomposition of NiSe2 during HER. Theoretical calculations suggested that the charge transfers from the Se site to Ni site during this evolution process, leading to an increased conductivity and a shifting up of d-band center, which is attributed to the enhanced activity. The generated NiSe phase acts as the “real” active species. Our work unravels the underlying phase transition of the electrocatalyst on reductive conditions in alkaline medium and highlights the significance of identifying the intrinsic active sites under realistic reaction conditions.	Jul 2020
	Transition metal migration can facilitate ionic diffusion in defect garnet based intercalation electrodes Nicholas H Bashian , Samantha Abdel-latif , Mateusz Zuba , Kent J. Griffith , Alex M. Ganose , Joseph W. Stiles , Shiliang Zhou , David O. Scanlon , Louis F. J. Piper , Brent Melot Acs Energy Letters DOI: 10.1021/acsenergylett.0c00376 Show Abstract ▼ Abstract: The importance of metal migration during multi-electron redox activity has been characterized, revealing a competing demand to satisfy bonding requirements and local strains in structures upon alkali intercalation. The local structural evolution required to accommodate intercalation in Y2(MoO4)3 and Al2(MoO4)3 has been contrasted by operando characterization methods, including X-ray absorption spectroscopy and diffraction, along with nuclear magnetic resonance measurements. Computational modeling further rationalized behavioral differences. The local structure of Y2(MoO4)3 was maintained upon lithiation while the structure of Al2(MoO4)3 underwent substantial local atomic rearrangements as the stronger ionic character of the bonds in Al2(MoO4)3 allowed Al to mix off its starting octahedral position to accommodate strain during cycling. However, this mixing was prevented in the more covalent Y2(MoO4)3 which accommodated strain through rotational motion of polyhedral subunits. Knowing that an increased ionic character can facilitate the diffusion of redox-inactive metals when cycling multi-electron electrodes offers a powerful design principle when identifying next-generation intercalation hosts.	Apr 2020
I09-Surface and Interface Structural Analysis	Quantifying the capacity contributions during activation of Li2MnO3 Jatinkumar Rana , Joseph K. Papp , Zachary Lebens-higgins , Mateusz Zuba , Lori A. Kaufman , Anshika Goel , Richard Schmuch , Martin Winter , M. Stanley Whittingham , Wanli Yang , Bryan D. Mccloskey , Louis F. J. Piper Acs Energy Letters DOI: 10.1021/acsenergylett.9b02799 Diamond Proposal Number(s): [22250] Show Abstract ▼ Abstract: Though Li2MnO3 was originally considered to be electrochemically inert, its observed activation has spawned a new class of Li-rich layered compounds that deliver capacities beyond the traditional transition-metal redox limit. Despite progress in our understanding of oxygen redox in Li-rich compounds, the underlying origin of the initial charge capacity of Li2MnO3 remains hotly contested. To resolve this issue, we review all possible charge compensation mechanisms including bulk oxygen redox, oxidation of Mn4+, and surface degradation for Li2MnO3 cathodes displaying capacities exceeding 350 mAh g–1. Using elemental and orbital selective X-ray spectroscopy techniques, we rule out oxidation of Mn4+ and bulk oxygen redox during activation of Li2MnO3. Quantitative gas-evolution and titration studies reveal that O2 and CO2 release accounted for a large fraction of the observed capacity during activation with minor contributions from reduced Mn species on the surface. These studies reveal that, although Li2MnO3 is considered critical for promoting bulk anionic redox in Li-rich layered oxides, Li2MnO3 by itself does not exhibit bulk oxygen redox or manganese oxidation beyond its initial Mn4+ valence.	Jan 2020
I13-2-Diamond Manchester Imaging	Morphological reversibility of modified Li-based anodes for next-generation batteries Fu Sun , Dong Zhou , Xin He , Markus Osenberg , Kang Dong , Libao Chen , Shilin Mei , Andre Hilger , Henning Markötter , Yan Lu , Shanmu Dong , Shashidhara Marathe , Christoph Rau , Xu Hou , Jie Li , Marian Cristian Stan , Martin Winter , Robert Dominko , Ingo Manke Acs Energy Letters DOI: 10.1021/acsenergylett.9b02424 Diamond Proposal Number(s): [18936] Show Abstract ▼ Abstract: Although a great variety of strategies to suppress Li dendrite have been proposed for lithium metal batteries (LMBs), a deeper understanding of the factors playing a crucial role during extended electrochemical cycling is often lacking. Herein, the morphological reversibility of the Li-based anode for next-generation batteries under three prevalent strategies, i.e., the use of Li–Al alloys, polymer coating, and anodic aluminum oxide (AAO) membrane attachment, has been sophisticatedly investigated by nondestructive visualization. The characterizations clearly capture the unprecedented morphological evolution of the Li-based anode during the electrochemical cycling. Furthermore, the results unambiguously indicate the formation of the “dead” electrochemically generated porous structures regardless of >99% cycling efficiency shown in Li symmetric cells in all three cell configurations. The results presented here shed light on further understanding of the morphological evolution of the Li anode under different scenarios, and it also enlightens us on new research activities that may assist in propelling the commercialization of LMBs.	Dec 2019
I07-Surface & interface diffraction	13.9% efficiency ternary nonfullerene solar cells featuring low-structural order Baocai Du , Renyong Geng , Wei Li , Donghui Li , Yuchao Mao , Mengxue Chen , Xue Zhang , Joel A. Smith , Rachel C. Kilbride , Mary E. O'kane , Dan Liu , David G. Lidzey , Weihua Tang , Tao Wang Acs Energy Letters DOI: 10.1021/acsenergylett.9b01630 Diamond Proposal Number(s): [22651] Show Abstract ▼ Abstract: The insufficient phase separation between polymer donors and non-fullerene acceptors (NFAs) featuring with low-structural orders disrupts efficient charge transport and increases charge recombination, consequently limits the maximum achievable power conversion efficiency (PCE) of organic solar cells (OSCs). Herein, an NFA IT-M has been added as the third component into the PBDB-T:m-INPOIC OSCs, and is shown to effectively tune the phase separation between donor and acceptor molecules, although all components in the ternary system exhibit low degrees of structural orders. The incorporation of 10 wt% IT-M into a PBDB-T:m-INPOIC binary host blend appreciably increases the length scale of phase separation, creating continuous pathways which increase and balance charge transport. This leads to an enhanced photovoltaic performance from 12.8% in the binary cell to 13.9% for the ternary cell with simultaneously improved open-circuit voltage, short-circuit current and fill factor. This work highlights the beneficial role of ternary components in controlling the morphology of the active layer for high performance OSCs.	Sep 2019
B18-Core EXAFS	Revealing the pH dependent activities and surface instabilities for Ni-based electrocatalysts during the oxygen evolution reaction Chunzhen Yang , Maria Batuk , Quentin Jacquet , Gwenaëlle Rousse , Wei Yin , Leiting Zhang , Joke Hadermann , Artem Abakumov , Giannantonio Cibin , Alan Chadwick , Jean-marie Tarascon , Alexis Grimaud Acs Energy Letters DOI: 10.1021/acsenergylett.8b01818 Diamond Proposal Number(s): [12559] Show Abstract ▼ Abstract: Multiple electrochemical processes are involved at the catalyst/electrolyte interface during the oxygen evolution reaction (OER). With the purpose of elucidating the complexity of surface dynamics upon OER, we systematically studied two Ni-based crystalline oxides (LaNiO3-δ and La2Li0.5Ni0.5O4) and compared them with the state-of-the-art Ni-Fe (oxy)hydroxide amorphous catalyst. Electrochemical measurements such as rotating ring disk electrode (RRDE) and electrochemical quartz microbalance microscopy (EQCM), coupled with a series of physical characterizations including transmission electron microscopy (TEM) and X-ray absorption spectroscopy (XAS) are conducted to unravel the exact pH effect on both the OER activity and the catalyst stability. We demonstrate that for Ni-based crystalline catalysts the rate for surface degradation depends on the pH and is greater than the rate for surface reconstruction. This behavior is unlike for amorphous Ni oxyhydroxide catalyst which is found more stable and pH independent.	Nov 2018
	Correlated polyhedral rotations in the absence of polarons during electrochemical insertion of lithium in ReO3 Nicholas H. Bashian , Shiliang Zhou , Mateusz Zuba , Alex M. Ganose , Joseph W. Stiles , Allyson Ee , David S. Ashby , David O. Scanlon , Louis F. J. Piper , Bruce S. Dunn , Brent C. Melot Acs Energy Letters DOI: 10.1021/acsenergylett.8b01179 Show Abstract ▼ Abstract: Understanding the structural transformations that materials undergo during the insertion and deinsertion of Li-ions is crucial for designing high performance intercalation hosts as these deformations can lead to significant capacity fade over time. Here we present a study of the metallic defect perovskite ReO3, with the goal of determining whether these distortions are driven by polaronic charge transport (i.e. the electrons and ions moving through the lattice in a coupled way) due to the semiconducting nature of most oxide hosts. Employing a range of techniques including galvanostatic/potentiometric electrochemical probes, operando X-ray diffraction, X-ray photoelectron spectroscopy, and density functional theory calculations we nd that the cubic structure of ReO3 experiences multiple phase changes involving the correlated twisting of rigid octahedral subunits during the insertion of two equivalents of Li-ions. This extensive rearrangement of the structure results in exceptionally poor long-term cyclability due to large strains that result within the structure, all in spite of the fact that the phase retains its metallic character for all values of Li content from ReO3 to Li2ReO3. These results suggest that phase transformations during alkali ion intercalation are the result of local strains in the lattice and not exclusively due to polaron migration.	Sep 2018

Publications Database

Search Results

You searched for all publications:

Search Again...

Subject Areas (check all that apply) select all

Instruments used to collect data (check all that apply) select all

Collaborations involved (check all that apply) select all

Diamond Offline Facilities used

Relevant Technical Areas (check all that apply) select all

Menu for Anonymous User