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While solid-state batteries are tantalizing for achieving improved safety and higher energy density, solid ion conductors currently available fail to satisfy the rigorous requirements for battery electrolytes and electrodes. Inorganic ion conductors allow fast ion transport, but their rigid and brittle nature prevents good interfacial contact and impedes device integration and stability.Conversely, flexible polymeric ion conductors provide better interfacial compatibility and mechanical tolerance, but suffer from inferior ionic conductivity (< 10 −5 S cm −1 at room temperature) due to the coupling of ion transport with the polymer chain motion 1-3 . In this work, we report a general design strategy for achieving one-dimensional (1D), high-performance polymer solid-state ion conductors through molecular channel engineering, which we demonstrate via Cu 2+ -coordination of cellulose nanofibrils. The cellulose nanofibrils by themselves are not ionic conductive; however, by opening the molecular channels between the cellulose chains through Cu 2+ coordination we are able to achieve a Li-ion conductivity as high as 1.5×10 −3 S cm −1 at room temperature-a record among all known polymer ion conductors. This improved conductivity is enabled by a unique Li + hopping mechanism that is decoupled from the polymer segmental motion. Also benefitted from such decoupling, the cellulose-based ion conductor demonstrates multiple advantages, including a high transference number (0.78 vs. 0.2-0.5 in other polymers 2 ), low activation energy (0.19 eV), and a wide electrochemical stability window (4.5 V) that accommodate both Li metal anode and high-voltage cathodes. Furthermore, we demonstrate this 1D ion conductor not only as a thin, high-conductivity solid-state electrolyte but also as an effective ion-conducting additive for the solid cathode, providing continuous ion transport pathways with a low percolation threshold, which allowed us to utilize the thickest LiFePO4 solidstate cathode ever reported for high energy density. This approach has been validated with other 3 polymers and cations (e.g., Na + and Zn 2+ ) with record-high conductivities, offering a universal strategy for fast single-ion transport in polymer matrices, with significance that could go far beyond safe, high-performance solid-state batteries.

Mitigating nitrogen oxide (NO x ) emissions is critical to tackle global warming and improve air quality. Conventional NO x abatement technologies for emission control suffer from a low efficiency at near ambient temperatures. Herein, we show an electrochemical pathway to reduce gaseous NO x that can be conducted at high reaction rates (400 mA cm–2) under ambient conditions. Various transition metals are evaluated for electrochemical reduction of NO and N2O to reveal the role of electrocatalyst in determining the product selectivity. Specifically, Cu is highly selective toward NH3 formation with >80% Faradaic efficiency in NO electroreduction. Furthermore, the partial pressure study of NO electroreduction revealed that a high NO coverage facilitates the N–N coupling reaction. In acidic electrolytes, the formation of NH3 is greatly favored, whereas the N2 production is suppressed. Additional mechanistic studies were conducted by using flow electrochemical mass spectrometry to gain further insights into reaction pathways. This work provides a promising avenue toward abating gaseous NO x emissions at ambient conditions by using renewable electricity.

Electrochemical conversion of carbon dioxide (CO2) to value-added chemicals has attracted much attention in recent years as a potential alternative to fossil resources. Although significant works have studied the influence of impurities in the electrolyte (e.g., metal ions), few studies have been performed to understand the influence of gaseous impurities in CO2 electroreduction. Herein, we study the effects of sulfur dioxide (SO2) on Ag-, Sn-, and Cu-catalyzed CO2 electrolysis in a flow-cell electrolyzer in near-neutral electrolyte, representing a broad range of CO2 reduction catalysts. We show that the presence of SO2 impurity reduces the efficiency of converting CO2 due to the preferential reduction of SO2. In the cases of Ag and Sn, the effect of SO2 impurity was reversible and the catalytic activities of both catalysts were recovered. On the contrary, a shift in selectivity toward formate accompanied by a suppression of multicarbon (C2+) products was observed on Cu catalyst, demonstrating that Cu is highly sensitive to SO2 impurity. Our results suggest that CO2 obtained from direct air capture technologies or biorefineries could be more suitable for Cu-catalyzed CO2 electrolysis as these CO2 sources would be relatively cleaner (SO2-free) than fossil-derived sources such as power plants and can be directly coupled with distributed renewable energy sources such as wind and solar.

Bimetallics are emerging as important materials that often exhibit distinct chemical properties from monometallics. However, there is limited access to homogeneously alloyed bimetallics because of the thermodynamic immiscibility of the constituent elements. Overcoming the inherent immiscibility in bimetallic systems would create a bimetallic library with unique properties. Here, we present a nonequilibrium synthesis strategy to address the immiscibility challenge in bimetallics. As a proof of concept, we synthesize a broad range of homogeneously alloyed Cu-based bimetallic nanoparticles regardless of the thermodynamic immiscibility. The nonequilibrated bimetallic nanoparticles are further investigated as electrocatalysts for carbon monoxide reduction at commercially relevant current densities (>100 mA cm−2), in which Cu0.9Ni0.1 shows the highest multicarbon product Faradaic efficiency of ~76% with a current density of ~93 mA cm−2. The ability to overcome thermodynamic immiscibility in multimetallic synthesis offers freedom to design and synthesize new functional nanomaterials with desired chemical compositions and catalytic properties.

catalysts exhibited a high sensitivity to the presence of SO 2 even at an extremely low concentration.

The electroreduction of carbon dioxide offers a promising avenue to produce valuable fuels and chemicals using greenhouse gas carbon dioxide as the carbon feedstock. Because industrial carbon dioxide point sources often contain numerous contaminants, such as nitrogen oxides, understanding the potential impact of contaminants on carbon dioxide electrolysis is crucial for practical applications. Herein, we investigate the impact of various nitrogen oxides, including nitric oxide, nitrogen dioxide, and nitrous oxide, on carbon dioxide electroreduction on three model electrocatalysts (i.e., copper, silver, and tin). We demonstrate that the presence of nitrogen oxides (up to 0.83%) in the carbon dioxide feed leads to a considerable Faradaic efficiency loss in carbon dioxide electroreduction, which is caused by the preferential electroreduction of nitrogen oxides over carbon dioxide. The primary products of nitrogen oxides electroreduction include nitrous oxide, nitrogen, hydroxylamine, and ammonia. Despite the loss in Faradaic efficiency, the electrocatalysts exhibit similar carbon dioxide reduction performances once a pure carbon dioxide feed is restored, indicating a negligible long-term impact of nitrogen oxides on the catalytic properties of the model catalysts.