|
|
Nuria
Tapia-Ruiz
,
A. Robert
Armstrong
,
Hande
Alptekin
,
Marco A.
Amores
,
Heather
Au
,
Jerry
Barker
,
Rebecca
Boston
,
William R
Brant
,
Jake M.
Brittain
,
Yue
Chen
,
Manish
Chhowalla
,
Yong-Seok
Choi
,
Sara I. R.
Costa
,
Maria
Crespo Ribadeneyra
,
Serena A
Cussen
,
Edmund J.
Cussen
,
William I. F.
David
,
Aamod V
Desai
,
Stewart A. M.
Dickson
,
Emmanuel I.
Eweka
,
Juan D.
Forero-Saboya
,
Clare
Grey
,
John M.
Griffin
,
Peter
Gross
,
Xiao
Hua
,
John T. S.
Irvine
,
Patrik
Johansson
,
Martin O.
Jones
,
Martin
Karlsmo
,
Emma
Kendrick
,
Eunjeong
Kim
,
Oleg V
Kolosov
,
Zhuangnan
Li
,
Stijn F L
Mertens
,
Ronnie
Mogensen
,
Laure
Monconduit
,
Russell E
Morris
,
Andrew J.
Naylor
,
Shahin
Nikman
,
Christopher A
O’keefe
,
Darren M. C.
Ould
,
Robert G.
Palgrave
,
Philippe
Poizot
,
Alexandre
Ponrouch
,
Stéven
Renault
,
Emily M.
Reynolds
,
Ashish
Rudola
,
Ruth
Sayers
,
David O.
Scanlon
,
S.
Sen
,
Valerie R.
Seymour
,
Begoña
Silván
,
Moulay Tahar
Sougrati
,
Lorenzo
Stievano
,
Grant S.
Stone
,
Chris I.
Thomas
,
Maria-Magdalena
Titirici
,
Jincheng
Tong
,
Thomas J.
Wood
,
Dominic S
Wright
,
Reza
Younesi
Open Access
Abstract: Increasing concerns regarding the sustainability of lithium sources, due to their limited availability and consequent expected price increase, have raised awareness of the importance of developing alternative energy-storage candidates that can sustain the ever-growing energy demand. Furthermore, limitations on the availability of the transition metals used in the manufacturing of cathode materials, together with questionable mining practices, are driving development towards more sustainable elements. Given the uniformly high abundance and cost-effectiveness of sodium, as well as its very suitable redox potential (close to that of lithium), sodium-ion battery technology offers tremendous potential to be a counterpart to lithium-ion batteries (LIBs) in different application scenarios, such as stationary energy storage and low-cost vehicles. This potential is reflected by the major investments that are being made by industry in a wide variety of markets and in diverse material combinations. Despite the associated advantages of being a drop-in replacement for LIBs, there are remarkable differences in the physicochemical properties between sodium and lithium that give rise to different behaviours, for example, different coordination preferences in compounds, desolvation energies, or solubility of the solid–electrolyte interphase inorganic salt components. This demands a more detailed study of the underlying physical and chemical processes occurring in sodium-ion batteries and allows great scope for groundbreaking advances in the field, from lab-scale to scale-up. This roadmap provides an extensive review by experts in academia and industry of the current state of the art in 2021 and the different research directions and strategies currently underway to improve the performance of sodium-ion batteries. The aim is to provide an opinion with respect to the current challenges and opportunities, from the fundamental properties to the practical applications of this technology.
|
Jul 2021
|
|
I11-High Resolution Powder Diffraction
|
Daniel S.
Firth
,
Samuel A.
Morris
,
Paul S.
Wheatley
,
Samantha E.
Russell
,
Alexandra M. Z.
Slawin
,
Daniel M.
Dawson
,
Alvaro
Mayoral
,
Maksym
Opanasenko
,
Miroslav
Polozij
,
Jiri
Cejka
,
Petr
Nachtigall
,
Russell E.
Morris
Abstract: The hydrothermal synthesis of a zeolite, with properties suitable for use in the ADOR (Assembly-Disassembly-Organisation-Reassembly) process, has been designed and a zeolite, called SAZ-1, successfully prepared. This zeolite has then been used as a parent in the ADOR process and two new daughter zeolites, IPC-15 and IPC-16, have been prepared. The X-ray powder diffraction patterns of the new zeolites match well those predicted using computational methods. The three materials, form an isoreticular series with decreasing pores size from 14-ring to 12-ring to 10-ring.
|
Jun 2017
|
|
I11-High Resolution Powder Diffraction
I15-Extreme Conditions
|
Diamond Proposal Number(s):
[10085]
Abstract: The disordered intermediate of the ADORable zeolite UTL has been structurally confirmed using the pair distribution function (PDF) technique. The intermediate, IPC-1P, is a disordered layered compound formed by the hydrolysis of UTL in 0.1 M hydrochloric acid solution. Its structure is unsolvable by traditional X-ray diffraction techniques. The PDF technique was first benchmarked against high-quality synchrotron Rietveld refinements of IPC-2 (OKO) and IPC-4 (PCR) – two end products of IPC-1P condensation that share very similar structural features. An IPC-1P starting model derived from density functional theory was used for the PDF refinement, which yielded a final fit of Rw = 18% and a geometrically reasonable structure. This confirms the layers do stay intact throughout the ADOR process and shows PDF is a viable technique for layered zeolite structure determination.
|
Aug 2016
|
|
I19-Small Molecule Single Crystal Diffraction
|
Diamond Proposal Number(s):
[24028]
Open Access
Abstract: The size of single crystals of the metal-organic framework CPO-27-Ni was incrementally increased through a series of modulated syntheses. A novel linker modulated synthesis using 2,5-dihydroxyterephthalic acid and the isomeric ligand 4,6-dihydroxyisophthalic acid yielded large single crystals of CPO-27-Ni (~70 µm). All materials proved high crystallinity and phase pure through powder X-ray diffraction, electron microscopy methods, thermogravimetric, and compositional analysis. For the first time single crystal structure analyses were carried out on CPO-27-Ni. High BET surface areas and nitric oxide (NO) release efficiencies were recorded for all materials. Large single crystals of CPO-27-Ni showed a prolonged NO release and proved suitable for in situ single crystal diffraction experiments to follow the NO adsorption. An efficient activation protocol was developed, leading to a dehydrated structure after just 4 h, which subsequently was NO-loaded, giving a first NO loaded single crystal structural model of CPO-27-Ni.
|
Mar 2021
|
|
I11-High Resolution Powder Diffraction
|
Open Access
Abstract: The assembly–disassembly–organization–reassembly (ADOR) process has been used to disassemble a parent zeolite with the UOV structure type and then reassemble the resulting layers into a novel structure, IPC-12. The structure of the material has previously been predicted computationally and confirmed in our experiments using X-ray diffraction and atomic resolution STEM-HAADF electron microscopy. This is the first successful application of the ADOR process to a material with porous layers.
|
Apr 2017
|
|
I11-High Resolution Powder Diffraction
|
Lauren N.
Mchugh
,
Matthew J.
Mcpherson
,
Laura J.
Mccormick
,
Samuel A.
Morris
,
Paul S.
Wheatley
,
Simon J.
Teat
,
David
Mckay
,
Daniel M.
Dawson
,
Charlotte E. F.
Sansome
,
Sharon E.
Ashbrook
,
Corinne A.
Stone
,
Martin W.
Smith
,
Russell E.
Morris
Abstract: Highly porous metal–organic frameworks (MOFs), which have undergone exciting developments over the past few decades, show promise for a wide range of applications. However, many studies indicate that they suffer from significant stability issues, especially with respect to their interactions with water, which severely limits their practical potential. Here we demonstrate how the presence of ‘sacrificial’ bonds in the coordination environment of its metal centres (referred to as hemilability) endows a dehydrated copper-based MOF with good hydrolytic stability. On exposure to water, in contrast to the indiscriminate breaking of coordination bonds that typically results in structure degradation, it is non-structural weak interactions between the MOF’s copper paddlewheel clusters that are broken and the framework recovers its as-synthesized, hydrated structure. This MOF retained its structural integrity even after contact with water for one year, whereas HKUST-1, a compositionally similar material that lacks these sacrificial bonds, loses its crystallinity in less than a day under the same conditions.
|
Aug 2018
|
|
I19-Small Molecule Single Crystal Diffraction
|
Diamond Proposal Number(s):
[29217]
Open Access
Abstract: Metal-organic frameworks (MOFs) are well known for their ability to adsorb various gases. The use of MOFs for the storage and release of biologically active gases, particularly nitric oxide (NO) and carbon monoxide (CO), has been a subject of interest. To elucidate the binding mechanisms and geometry of these gases, an in situ single crystal X-ray diffraction (scXRD) study using synchrotron radiation at Diamond Light Source has been performed on a set of MOFs that display promising gas adsorption properties. NO and CO, were introduced into activated Ni-CPO-27 and the related Co-4,6-dihydroxyisophthalate (Co-4,6-dhip). Both MOFs show strong binding affinity towards CO and NO, however CO suffers more from competitive co-adsorption of water. Additionally, we show that morphology can play an important role in the ease of dehydration for these two systems.
|
Mar 2023
|
|
I11-High Resolution Powder Diffraction
|
Samuel A.
Morris
,
Giulia P. M.
Bignami
,
Yuyang
Tian
,
Marta
Navarro
,
Daniel S.
Firth
,
Jiří
Čejka
,
Paul S.
Wheatley
,
Daniel M.
Dawson
,
Wojciech A.
Slawinski
,
David S.
Wragg
,
Russell E.
Morris
,
Sharon E.
Ashbrook
Abstract: The assembly–disassembly–organization–reassembly (ADOR) mechanism is a recent method for preparing inorganic framework materials and, in particular, zeolites. This flexible approach has enabled the synthesis of isoreticular families of zeolites with unprecedented continuous control over porosity, and the design and preparation of materials that would have been difficult—or even impossible—to obtain using traditional hydrothermal techniques. Applying the ADOR process to a parent zeolite with the UTL framework topology, for example, has led to six previously unknown zeolites (named IPC-n, where n = 2, 4, 6, 7, 9 and 10). To realize the full potential of the ADOR method, however, a further understanding of the complex mechanism at play is needed. Here, we probe the disassembly, organization and reassembly steps of the ADOR process through a combination of in situ solid-state NMR spectroscopy and powder X-ray diffraction experiments. We further use the insight gained to explain the formation of the unusual structure of zeolite IPC-6.
|
Apr 2017
|
|
I11-High Resolution Powder Diffraction
|
Abstract: PC-12 zeolite is the first member of ADOR family produced by the structural transformation of UOV. The details of UOV rearrangement were studied to determine the influence of properties of parent zeolite and treatment conditions on the outcome of IPC-12 formation. It was established that incomplete disassembly of UOV can be caused by insufficient lability of interlayer connectivity in parent material possessing Si-enriched D4Rs or by inhibition of hydrolysis by diluted acid at high temperature. The impacts of specific interactions of the framework with anions on controllable breaking of interlayer connectivity as well as the conditions of the treatment at low pH (< –1) on the characteristics of produced IPC-12 were found to be negligible. Concentration of acid significantly influences the extent and even the direction of UOV transformation. Layers disassembly is inhibited in 1 – 4 M acid solutions, complete hydrolysis to layered precursor can be achieved in 0.1 M, while application of 12 M solution lead to direct formation of IPC-12. Layers reassembly followed using in situ XRD measurement with synchrotron source was found to be gradual process starting already at 40 °C and completing at 200 – 220 °C.
|
Dec 2017
|
|
I11-High Resolution Powder Diffraction
|
Phoebe K.
Allan
,
Paul S.
Wheatley
,
David
Aldous
,
M. Infas
Mohideen
,
Chiu
Tang
,
Joseph A.
Hriljac
,
Ian L.
Megson
,
Karena W.
Chapman
,
Guy
De Weireld
,
Sebastian
Vaesen
,
Russell E.
Morris
Abstract: Hydrogen sulfide is an extremely toxic gas that is also of great interest for biological applications when delivered in the correct amount and at the desired rate. Here we show that the highly porous metal-organic frameworks with the CPO-27 structure can bind the hydrogen sulfide relatively strongly, allowing the storage of the gas for at least several months. Delivered gas is biologically active in preliminary vasodilation studies of porcine arteries, and the structure of the hydrogen sulfide molecules inside the framework has been elucidated using a combination of powder X-ray diffraction and pair distribution function analysis.
|
Mar 2012
|
|
