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Reduced graphene-oxide (RGO)-based electrodes in supercapacitors deliver high energy/power capacities compared to typical nanoporous carbon materials. However, extensive critical analysis of literature reveals enormous discrepancies (up to 250 F g-1 ) in the reported capacitance (variation of 100-350 F g-1 ) of RGO materials synthesized under seemingly similar methods, inhibiting an understanding of capacitance variation. Here, the key factors that control the capacitance performance of RGO electrodes are demonstrated by analyzing and optimizing various types of commonly applied electrode fabrication methods. Beyond usual data acquisition parameters and oxidation/reduction properties of RGO, a substantial difference of more than 100% in capacitance values (with change from 190 ± 20 to 340 ± 10 F g-1 ) is found depending on the electrode preparation method. For this demonstration, ≈40 RGO-based electrodes are fabricated from numerous distinctly different RGO materials via typically applied methods of solution (aqueous and organic) casting and compressed powders. The influence of data acquisition conditions and capacitance estimation practices are also discussed. Furthermore, by optimizing electrode processing method, a direct surface area governed capacitance relationship for RGO structures is revealed.

Metal-organic frameworks/zeolitic imidazolate frameworks (MOFs/ZIFs) and their post-synthesis modified nanostructures, such as oxides, hydroxides, and carbons have generated significant interest for electrocatalytic reactions. In this work, a high and durable oxygen evolution reaction (OER) performance directly from bimetallic Zn100-x Cox -ZIF samples is reported, without carrying out high-temperature calcination and/or carbonization. ZIFs can be reproducibly and readily synthesized in large scale at ambient conditions. The bimetallic ZIFs show a systematic and gradually improved OER activity with increasing cobalt concentration. A further increase in OER activity is evidenced in ZIF-67 polyhedrons with controlled particle size of 50 %, OER activity is obtained with ZIF-67/carbon black, which shows a low overpotential of approximately 320 mV in 1.0 m KOH electrolyte. Such activity is comparable to or better than numerous MOF/ZIF-derived electrocatalysts. The optimized ZIF-67 sample also exhibits increased activity and durability over 24 h, which is attributed to an in situ developed active cobalt oxide/oxyhydroxide related nanophase.

We propose a new synthetic route towards nanoporous functional carbon materials based on salt templating with pore-padding approach (STPP). STPP relies on the use of a pore-padding agent that undergoes an initial polymerisation/ condensation process prior to the formation of a solid carbon framework. The pore-padding agent allows tailoring hierarchically the pore-size distribution and controlling the amount of heteroatom (nitrogen in this case) functionalities as well as the type of nitrogen (graphitic, pyridinic, oxides of nitrogen) incorporated within the carbon framework in a single-step-process. Our newly developed STPP method offers a unique pathway and new design principle to create simultaneously high surface area, microporosity, functionality and pore hierarchy. The functional carbon materials produced by STPP showed a remarkable CO2/N2 selectivity. At 273 K, a carbon with only micropores offered an exceptionally high CO2 adsorption capacity whereas a carbon with only mesopores showed promising CO2-philicity with high CO2/N2 selectivity in the range of 46–60 %, making them excellent candidates for CO2 capture from flue gas or for CO2 storage.

Nanoporous carbons (NPCs) with engineered specific pore sizes and sufficiently high porosities (both specific surface area and pore volume) are necessary for storing energy in the form of electric charges and molecules. Herein, NPCs, derived from biomass pine‐cones, coffee‐grounds, graphene‐oxide and metal‐organic frameworks, with systematically increased pore width ( 50 Wh kg−1 at high power density, 1000 W kg−1) are achieved to form the highest reported values among the range of carbons in the literature. The noteworthy energy storage performance of the NPCs for all five cases (CO2, H2, H2O, and capacitance in aqueous and organic electrolytes) is highlighted by direct comparison to numerous existing porous solids. A further analysis on the specific pore type governed physisorption capacities is presented.

The room temperature synthesis of perovskite nanocrystals (NCs) is typically achieved by employing a ligand‐assisted reprecipitation (LARP) method, which can be handled in air, and its products are comparable to what is obtained using the traditional hot‐injection method. However, the LARP method typically requires the use of coordinating polar solvents such as dimethylformamide, which are not appropriate for large‐scale production due to toxicity concerns and can also degrade or form defective perovskite NCs. Herein, an amine and oleic‐acid‐free room temperature synthesis of lead bromide perovskite NCs is reported that uses a combination of trioctylphosphine oxide and diisooctylphosphinic acid ligands. This combination of ligands provides a stable platform for the polar‐solvent‐free synthesis in air of fully inorganic CsPbBr3 (fwhm ≈ 14 nm, emission = 519 nm) and hybrid organic‐inorganic FAPbBr3 (fwhm ≈ 19 nm) NCs with photoluminescence emission between 530 and 535 nm, which is in line with the Rec. 2020 color standards. In addition, it is shown that compared to a traditionally used ligand combination, phosphine ligands can be easily removed from the surface of the NCs, which is important for the future development of this technology in optoelectronic devices.

In article number https://doi.org/10.1002/advs.201901517, Srinivas Gadipelli and co‐workers present direct evidence of carbon nanoparticle size–dependent electrochemical activity for the supercapacitors and oxygen reduction reaction. For this, the carbon polyhedrons with size between few tens of nanometers to microns are designed from a zeolitic imidazolate framework (ZIF‐8), and all other parameters, such as surface area, microporosity, pore‐size distribution, nitrogen‐doping and graphitization are maintained identically.

Carbon monoliths of ultrahigh pore volume (5.35 cm(3) g(-1) ) and high surface area (2700 m(2) g(-1) ) accommodate a record high level of amine(tetraethylenepentamine), up to 5 g g(-1) within its hierarchically networked micro-/mesopores over a wide range. Thus, this solid-amine@carbon shows exceptional CO2 sorption and stable cyclic capacities at simulated flue-gas conditions.

A highly effective and facile synthesis route is developed to create and tailor metal-decorated and nitrogen-functionalized active microporous carbon materials from ZIF-8. Clear metal- and pyrrolic-N-induced enhancements of the cyclic CO2 uptake capacities and binding energies are achieved, particularly at a much lower carbonization temperature of 700 °C than those often reported (1000 °C). The high-temperature carbonization can enhance the porosity but only at the expense of considerable losses of sample yield and metal and N functional sites. The findings are comparatively discussed with carbons derived from metal–organic frameworks (MOFs) reported previously. Furthermore, the porosity of the MOF-derived carbon is critically dependent on the structure of the precursor MOF and the crystal growth. The current strategy offers a new and effective route for the creation and tuning of highly active and functionalized carbon structures in high yields and with low energy consumption.

Metal–organic framework–derived carbon nanostructures have generated significant interest in electrochemical capacitors and oxygen/hydrogen catalysis reactions. However, they appear to show considerably varied structural properties, and thus exhibit complex electrochemical–activity relationships. Herein, a series of carbon polyhedrons of different sizes, between 50 nm and µm, are synthesized from zeolitic imidazolate frameworks, ZIF‐8 (ZIF‐derived carbon polyhedrons, ZDCPs) and their activity is studied for capacitance and the oxygen reduction reaction (ORR). Interestingly, a well‐correlated performance relationship with respect to the particle size of ZDCPs is evidenced. Here, the identical structural features, such as specific surface area (SSA), microporosity, and its distribution, nitrogen doping, and graphitization are all strictly maintained in the ZDCPs, thus allowing identification of the effect of particle size on electrochemical performance. Supercapacitors show a capacity enhancement of 50 F g−1 when the ZDCPs size is reduced from micrometers to ≤200 nm. The carbonization further shows a considerable effect on rate capacitance—ZDCPs of increased particle size lead to drastically reduced charge transportability and thus inhibit their performance for both the charge storage and the ORR. Guidelines for the capacitance variation with respect to the particle size and SSA in such carbon nanostructures from literature are presented., Carbon‐based nanostructures are indispensable for supercapacitors, fuel cells, and batteries. Advancement in this area requires critical understanding of the form and function. Here, a well‐correlated relationship is demonstrated for the performance of supercapacitors and the oxygen reduction reaction with respect to particle size of metal–rganic frameworks–derived carbon. Surface area, pore‐size distribution, nitrogen doping, and graphitization are all maintained identical.

The addition of cations to TiO2 photoelectrodes is routinely accepted as a route to enhance the performance of conventional n‐i‐p solar cells. However, this is typically achieved in multiple steps or by the incorporation of expensive and hydroscopic cationic precursors such as lithium bis(trifluoromethanesulfonyl)imide. In addition, it is often unclear as to whether the incorporation of such cation sources is inducing “doping” or simply transformed into cationic oxides on the surface of the photoelectrodes. In this study, TiO2 nanofibers were produced through a simple electrospinning technique and modified by introducing lithium and lanthanum precursors in one step. Our results show that the addition of both cations caused minimal substitutional or interstitial doping of TiO2. Brunauer‐Emmett‐Teller measurements showed that lanthanum‐treated TiO2 nanofibers had an increase in surface area, which even exceeded that of TiO2 P25 nanoparticles. Finally, treated and untreated TiO2 nanofibers were used in n‐i‐p solar cells. Photovoltaic characteristics revealed that lanthanum treatment was beneficial, whereas lithium treatment was found to be detrimental to the device performance for both dye‐sensitized and perovskite solar cells. The results discuss new fundamental understandings for two of the commonly incorporated cationic dopants in TiO2 photoelectrodes, lithium and lanthanum, and present a significant step forward in advancing the field of materials chemistry for photovoltaics.

On page 4903, S. Gadipelli, Z. Guo, and co-workers describe solidamine@carbon monoliths of ultrahigh hierarchical pore volume (5.35 cm(3) g(-1) ) that have a wide-range pore-size distribution (up to 50 nm) and high specific surface area (2700 m(2) g(-1) ). They also show exceptional CO2 sorption kinetics and stable cyclic capacities (over 200 mg g(-1) ) at simulated flue-gas conditions (75 °C and 15% CO2 , humidified and balanced with N2 ).