Search

Stimuli-responsive behaviors of flexible metal-organic frameworks (MOFs) make these materials promising in a wide variety of applications such as gas separation, drug delivery, and molecular sensing. Considerable efforts have been made over the last decade to understand the structural changes of flexible MOFs in response to external stimuli. Uniform pore deformation has been used as the general description. However, recent advances in synthesizing MOFs with non-uniform porous structures, i.e. with multiple types of pores which vary in size, shape, and environment, challenge the adequacy of this description. Here, we demonstrate that the CO2-adsorption-stimulated structural change of a flexible MOF, ZIF-7, is induced by CO2 migration in its non-uniform porous structure rather than by the proactive opening of one type of its guest-hosting pores. Structural dynamics induced by guest migration in non-uniform porous structures is rare among the enormous number of MOFs discovered and detailed characterization is very limited in the literature. The concept presented in this work provides new insights into MOF flexibility.

Widespread access to greener energy is required in order to mitigate the effects of climate change. A significant barrier to cleaner natural gas usage lies in the safety/efficiency limitations of storage technology. Despite highly porous metal-organic frameworks (MOFs) demonstrating record-breaking gas-storage capacities, their conventionally powdered morphology renders them non-viable. Traditional powder shaping utilising high pressure or chemical binders collapses porosity or creates low-density structures with reduced volumetric adsorption capacity. Here, we report the engineering of one of the most stable MOFs, Zr-UiO-66, without applying pressure or binders. The process yields centimetre-sized monoliths, displaying high microporosity and bulk density. We report the inclusion of variable, narrow mesopore volumes to the monoliths' macrostructure and use this to optimise the pore-size distribution for gas uptake. The optimised mixed meso/microporous monoliths demonstrate Type II adsorption isotherms to achieve benchmark volumetric working capacities for methane and carbon dioxide. This represents a critical advance in the design of air-stable, conformed MOFs for commercial gas storage.

et al., Large datasets are now ubiquitous as technology enables higher-throughput experiments, but rarely can a research field truly benefit from the research data generated due to inconsistent formatting, undocumented storage or improper dissemination. Here we extract all the meaningful device data from peer-reviewed papers on metal-halide perovskite solar cells published so far and make them available in a database. We collect data from over 42,400 photovoltaic devices with up to 100 parameters per device. We then develop open-source and accessible procedures to analyse the data, providing examples of insights that can be gleaned from the analysis of a large dataset. The database, graphics and analysis tools are made available to the community and will continue to evolve as an open-source initiative. This approach of extensively capturing the progress of an entire field, including sorting, interactive exploration and graphical representation of the data, will be applicable to many fields in materials science, engineering and biosciences., Open access funding provided by Helmholtz-Zentrum Berlin für Materialien und Energie GmbH., The core funding of the project has been received from the European Union’s Horizon 2020 research and innovation programme under grant agreement no. 787289. We acknowledge the following sources for individual funding. Cambridge India Ramanujan Scholarship, China Scholarship Council, Deutscher Akademischer Austauschdienst (DAAD), EPSRC (grant no. EP/S009213/1), European Union’s Horizon 2020 research and innovation programme (grant no. 764787, EU Project ‘MAESTRO’), (grant no. 756962, ERC Project ‘HYPERION’), (grant no. 764047, EU Project ‘ESPResSo’ and grant no. 850937), GCRF/EPSRC SUNRISE (EP/P032591/1), German Federal Ministry for Education and Research (BMBF), HyPerFORME, NanoMatFutur (grant no. 03XP0091). PEROSEED (ZT-0024), Helmholtz Energy Materials Foundry, The Helmholtz Innovation Laboratory HySPRINT. BMBF (grant nos. 03SF0540, 03SF0557A), HyPerCells graduate school, Helmholtz Association, Helmholtz International Research School (HI-SCORE), the Erasmus programme (CDT-PV, grant no. EP/L01551X/1), the European Union’s Horizon 2020 research and innovation programme (Marie Skłodowska-Curie grant agreement nos. 841386, 795079 and 840751), Royal Society University Research Fellowship (grant no. UF150033). SNaPSHoTs (BMBF), SPARC II, German Research Foundation (DFG, grant no. SPP2196), The National Natural Science Foundation of China (grant no. 51872014), the Recruitment Programme of Global Experts, Fundamental Research Funds for the Central Universities and the ‘111’ project (grant no. B17002), the US Department of Energy’s Office of Energy Efficiency and Renewable Energy under Solar Energy Technologies Office (SETO) agreement no. DE-EE0008551, the Colombia Scientific Programme in the framework of the call Ecosistema Cientifíco (Contract no. FP44842-218-2018), the committee for the development of research (CODI) of the Universidad de Antioquia (grant no. 2017-16000), Spanish MINECO (Severo Ochoa programme, grant no. SEV‐2015‐0522), the Swedish research council (VR, grant no. 2019-05591) and the Swedish Energy Agency (grant no. 2020-005194).