Slowing climate change requires overcoming inertia in political, technological, and geophysical systems. Of these, only geophysical warming commitment has been quantified. We estimated the commitment to future emissions and warming represented by existing carbon dioxide–emitting devices. We calculated cumulative future emissions of 496 (282 to 701 in lower- and upper-bounding scenarios) gigatonnes of CO 2 from combustion of fossil fuels by existing infrastructure between 2010 and 2060, forcing mean warming of 1.3°C (1.1° to 1.4°C) above the pre-industrial era and atmospheric concentrations of CO 2 less than 430 parts per million. Because these conditions would likely avoid many key impacts of climate change, we conclude that sources of the most threatening emissions have yet to be built. However, CO 2 -emitting infrastructure will expand unless extraordinary efforts are undertaken to develop alternatives.

Future CO2 Emissions and Climate Change from Existing Energy Infrastructure

The field of metal–organic frameworks (MOFs) has been incorrectly believed to be purely crystalline. However, non-crystalline MOFs (amorphous MOFs, MOF liquids, and MOF glasses) are starting to emerge as alternative materials, beyond the dictatorial domain of crystalline MOFs. Non-crystalline MOFs present many opportunities, either as novel functional materials themselves, or as vehicles to create other materials. In this extensive Review, we describe the two approaches to preparing amorphous MOFs: (1) the amorphization of crystalline MOFs and (2) the direct synthesis. Special attention is paid to the relationship between preparation method, properties and applications of amorphous MOFs. We also explore the field of MOF liquids and their applications, centering our attention to the phenomenon of melting. Finally, MOF glasses are explained. We highlight the properties and applications of the MOF glasses that are not usually found in crystalline MOFs. New related glass materials such as MOF-blends, flux melted MOFs, MOF crystal-glass composites, MOF and inorganic glass composites, and MOF glass membranes are also reviewed. We conclude the fields of amorphous MOFs, MOF liquids, and MOF glasses by presenting our thoughts on the possible future research directions.

Metal–organic frameworks (MOFs) beyond crystallinity: amorphous MOFs, MOF liquids and MOF glasses

Significance The combined radical and nonradical reactions induced by peroxymonosulfate (PMS) activation can promise deep mineralization and selective removal of micropollutants from complex wastewater. However, nonhomogeneous metal-based catalysts with single active sites lead to a low efficiency of electron cycling for both radical and nonradical generation. In this study, asymmetric Co–O–Bi sites were constructed to achieve rapid electron cycling while achieving site synergy, thus effectively activating PMS to generate radicals and nonradicals. The presence of asymmetric sites can tune and optimize the catalytic performance through structural modulation, which can effectively remove and mineralize micropollutants from organic and inorganic compounds under the environmental background.

Generating dual-active species by triple-atom sites through peroxymonosulfate activation for treating micropollutants in complex water

Rare-earth (RE)-based transition metal oxides (TMO) are emerging as a frontier towards oxygen evolution reaction (OER), yet the knowledge regarding their electrocatalytic mechanism and active sites is very limited. Herein, we successfully design and synthesize atomically dispersed Ce on CoO by an effective plasma (P)-assisted strategy as a model (P-Ce SAs@CoO) to investigate the origin of OER performance in RE-TMO systems. The P-Ce SAs@CoO exhibits favorable performance with an overpotential of only 261 mV at 10 mA cm-2 and robust electrochemical stability, superior to individual CoO. X-ray absorption spectroscopy and in-situ electrochemical Raman spectroscopy uncover that the Ce-induced electron redistribution inhibits Co-O bond breakage in the Co-O-Ce unit site. Theoretical analyses demonstrate that the gradient orbital coupling reinforces the Co-O covalency of Ce(4f)-O(2p)-Co(3d) unit active site with an optimized Co-3d-eg occupancy, which can balance the adsorption strength of intermediates and in turn reach the apex of the theoretical OER maximum, in excellent agreement with experimental observations. We believe the establishment of this Ce-CoO model can set a basis for the mechanistic understanding and structural design of high-performance RE-TMO catalysts. This article is protected by copyright. All rights reserved.

Reinforce the Co-O Covalency via Ce(4f)-O(2p)-Co(3d) Gradient Orbital Coupling for High-efficiency Oxygen Evolution.

Regulating intermediates through elaborating catalyst design to control reaction direction is crucial for promoting the selectivity of electrocatalytic CO 2 -to-CH 4 . M-C (M = metal) bonds are particularly important for tuning multi-electron reaction, however, its construction in nanomaterials is challenging. Here, via rational design of in-situ anchoring Cu SAs (single atoms) on the unique platform graphdiyne, we firstly realize the construction of chemical bond Cu-C (GDY). In-situ Raman spectroelectrochemistry and DFT calculations confirm due to the fabrication of Cu-C bond, during CO 2 reduction, the formation of *OCHO intermediates is dominant rather than *COOH on Cu atoms, facilitating the formation of CH 4 . Therefore, we find that constructing Cu-C bond in Cu SAs/GDY can supply efficient charge transfer channel, but most importantly control the reaction intermediates and guide a more facile reaction pathway to CH 4 , thereby significantly boost its catalytic performance. This work provides new insights on enhancing the selectivity for CO 2 RR at atomic level.

Constructing Cu-C Bond in Graphdiyne-Regulated Cu Single Atom Electrocatalyst for CO2 Reduction to CH4.

Developing non-noble catalysts with superior activity and durability for oxygen evolution reaction (OER) in acidic media is paramount for hydrogen production from water. Still, challenges remain due to the inadequate activity and stability of the OER catalyst. Here, we report a cost-effective and stable manganese oxybromide (Mn7.5O10Br3) catalyst exhibiting an excellent OER activity in acidic electrolytes, with an overpotential of as low as 295 ± 5 mV at a current density of 10 mA cm-2. Mn7.5O10Br3 maintains good stability under operating conditions for at least 500 h. In situ Raman spectroscopy, X ray absorption near edge spectroscopy, and density functional theory calculations confirm that a self-oxidized surface with enhanced electronic transmission capacity forms on Mn7.5O10Br3 and is responsible for both the high catalytic activity and long-term stability during catalysis. The development of Mn7.5O10Br3 as an OER catalyst provides crucial insights into the design of non-noble metal electrocatalysts for water oxidation. 

/pdf/efficient-and-stable-noble-metal-free-catalyst-for-acidic-1ocsh18i.pdf

Efficient and stable noble-metal-free catalyst for acidic water oxidation

Using only low-cost materials to achieve a solar-to-hydrogen (STH) efficiency of over 20% for solar water splitting systems is still a major challenge for realizing the practical feasibility of photoelectrochemical (PEC) hydrogen production technology. Utilizing the electrochemical instability of some metal organic framework ligands is a promising strategy to solve the problem of difficulty in controlling the degree of electrochemical self-reconstruction and obtaining high-performance water oxidation catalysts. Here, a monolithic perovskite/silicon tandem solar cell was used for highly efficient standalone solar water splitting. A self-reconstructed NiCoFe-based hydroxide nanosheet electrocatalyst was shown to exhibit remarkable oxygen evolution reaction performance with an overpotential of 191 mV at 10 mA cm−2. Upon pairing with the reported state-of-the-art hydrogen evolution reaction catalyst NiMo4/MnO3−X and a monolithic perovskite/silicon tandem solar cell, an unprecedented STH efficiency of 21.32% was achieved for the unbiased solar water splitting system. This low-cost high-efficiency solar water-splitting system will contribute to realizing the practical applications of PEC hydrogen production technology.

An over 20% solar-to-hydrogen efficiency system comprising a self-reconstructed NiCoFe-based hydroxide nanosheet electrocatalyst and monolithic perovskite/silicon tandem solar cell

Photovoltaic hydrogen production from seawater is of great significance. Challenges of solar-driven seawater electrolysis, for example, competing among chlorine evolution reactions, chloride corrosion, and catalyst poisoning, seriously restrict the development of this technology. In this paper, we report a two-dimensional nanosheet quaternary metal hydroxide catalyst composed of Ni, Fe, Cr, and Mo elements. By in situ electrochemical activation, a partial Mo element was leached and morphologically transformed in the catalyst. The higher metal valence states and many O vacancies were obtained, providing excellent catalytic activity and corrosion resistance in overall alkaline seawater electrolysis operating at an industrial-required current density of 500 mA cm-2 over 1000 h under 1.82 V low voltages at room temperature. The floating solar seawater splitting device shows a 20.61 ± 0.77% efficiency of solar energy to hydrogen (STH). This work demonstrates the development of efficient solar seawater electrolysis devices and potentially promotes research on clean energy conversion.

Floating Seawater Splitting Device Based on NiFeCrMo Metal Hydroxide Electrocatalyst and Perovskite/Silicon Tandem Solar Cells.

Micro-Electrode with Fast Mass Transport for Enhancing Selectivity of Carbonaceous Products in Electrochemical CO2 Reduction

High-Performance and Stable Perovskite-Based Photoanode Encapsulated by Blanket-Cover Method

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