hinder the practical deployment of Li metal batteries. Thus far, various emerging strategies, including electrolyte optimization, [2] solid electrolyte application, [3] and artificial protective layer construction, [4] have been proposed to stabilize SEI. These strategies have achieved remarkable electrochemical performances and provided perspectives for developing long lifespan Li metal batteries. Regrettably, most of them were conducted in a coin cell setting. The resulted from different test conditions make it exceedingly difficult to compare the developed materials or concepts for practical application. [5] In real high-energy Li metal batteries, any minor defects (such as Li dendrites, interface parasitic reactions, and volume expansion) will be aggravated, leading to unstable cycle performance. In particular, when the coin cell is magnified to the pouch cell, it will be accompanied by some unpredictable problems. [6] For example, cell gassing, which is absolutely neglected in typical coin cells but turns into a new, inextricable problem in high-energy Li metal batteries. Gassing is a common phenomenon in other battery systems (such as lead-acid batteries, zinc-air batteries, and lithium titanate-based batteries) and has been studied in depth. [7] However, the gassing of Li metal batteries is often overlooked and has not attracted enough attention. It can be predicted that the gassing problem will be an inevitable topic in the future development of Li metal batteries. Generally, highly active Li metal reacts spontaneously with organic electrolyte to form an SEI layer. [8] Unfortunately, this passivated SEI film (commonly inhomogeneous, low modulus, and poor stability) hardly regulates uniform nucleation and growth of Li and suppresses interfacial parasitic reactions between Li metal and electrolyte, causing severe Li dendrites and gassing behavior, which have a considerable impact on the cycle life of high-energy Li metal batteries (Figure 1a). Hence, constructing a stable and cell-level SEI film to extend the cycle life in practical high-energy Li metal batteries is urgently needed.Here, we constructed an efficient multifunctional silanization interface (MSI) on the Li metal anode surface for highenergy Li metal pouch cells (Figure 1b). Contrasted with the original SEI film, MSI simultaneously possesses the properties of homogenizing Li-ion flux, high modulus, and high stability. The pouch cell assembled with the MSI protected Li metal anode (MSI-Li), high-area capacity LiNi 0.5 Co 0.2 Mn 0.3 O 2 cathode Lithium (Li) metal has attracted unprecedented attention as the ultimate anode material for future rechargeable batteries, but the electrochemical behavior (such as Li dendrites and gassing problems) in real Li metal pouch cells has received little attention. To achieve realistic high-energy Li metal batteries, the designed solid electrolyte interface to suppress both Li dendrites and catastrophic gassing problems is urgently needed at cell level. Here, an efficient multifunctional silanization interfac...

Lithium carbon dioxide (Li-CO 2 ) batteries deliver a theoretical energy density of 1876 W h kg −1 in terms of effective utilization of greenhouse gases. This battery system is considered to be an encouraging electrochemical energy storage device and a promising alternative to Li-ion batteries. However, the main drawback of Li-CO 2 batteries is their accumulative discharge product of Li 2 CO 3 /C, which leads to large overpotential and poor cycling performance. Thus, specific and efficient catalysts must be explored to enhance the decomposition of Li 2 CO 3 /C. Single-atom catalysts (SACs) are regarded as promising heterogeneous catalysts owing to their maximized utilization of metal atoms and strong interfacial electronic interactions. Herein, single-metal atoms of Fe, Co, and Ni uniformly anchored on N-doped reduced graphene oxide (rGO), designated as Fe 1 /N-rGO, Co 1 /N-rGO, and Ni 1 / N-rGO, respectively, are designed and fabricated to investigate their catalytic activity toward the decomposition of Li 2 CO 3 /C. Among them, Fe 1 /N-rGO delivers a high discharge capacity of 16,835 mA h g −1 at 100 mA g −1 and maintains stability for more than 170 cycles with a discharge voltage of 2.30 V at 400 mA g −1 . Therefore, this catalysts are overwhelmingly superior to other types. This work reveals the advances of SACs in Li-CO 2 batteries and offers an effective method for realizing high-performance Li-CO 2 batteries.

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sluggish redox kinetics of soluble lithium polysulfides (LiPSs) transforming into solid discharge products Li 2 S leads to the undesirable accumulation and shuttling of LiPSs, resulting in low actual specific energy density, rapid capacity decay, and poor rate performance. [4][5][6] Therefore, enhancing the electrochemical reaction kinetics is the key to achieving the practical application of high specific energy Li-S batteries.To conquer this fatal challenge, the electrocatalytic strategy has been addressed to ameliorate the LiPSs redox kinetics. [7][8][9] So far, various electrocatalysts have been explored to improve the kinetics of LiPSs redox reaction process. It is worth noting that these electrocatalysts can be mainly divided into heterogeneous and homogeneous electrocatalysts in terms of their phase states. [10] The heterogeneous electrocatalysts, such as metals, metal compounds (e.g., metal oxides, sulfides, nitrides, etc.), heterostructures, single-atom catalysts, etc., have been applied to promote sulfur redox kinetics mainly by their strong anchoring effect and LiPSs transformation ability. [11][12][13] For example, Arava and his colleagues first introduced Pt and Ni to Li-S cells, which consciously promoted electrochemical performance and opened the era of metal-based electrocatalysts for Li-S batteries. [14] However, the heterogeneous electrocatalysts are restricted to specific catalytic sites and easily deactivated due to the undesirable coverage of solid sulfides, which cannot guarantee the long-term operation of batteries. Moreover, recently, homogeneous electrocatalysts, the extrinsic redox mediators (e.g., quinones, organopolysulfides, etc.), are introduced to regulate LiPSs reduction route through customized chemical reactions, while the practical application of this kind of electrocatalyst is impeded by its low chemical stability and possible shuttle effect. [15][16][17] The two electrocatalytic strategies mentioned above provide new perspectives to address the issue of LiPSs shuttling and encourage the exploration of novel electrocatalysts with high and long-term stable catalytic activity.Gallium-based liquid metal has become research hotspots in various physical and chemical fields due to their melting points below room temperature as well as high metallic conductivity, which have expedited the wide applications in soft electronics, robotics engineering, and catalysis technology. [18][19][20][21] On one hand, excitingly, the liquid property with abundant Designing efficient electrocatalysts with high electroconductivity, strong chemisorption, and superior catalytical efficiency to realize rapid kinetics of the lithium polysulfides (LiPSs) conversion process is crucial for practical lithium-sulfur (Li-S) battery applications. Unfortunately, most current electrocatalysts cannot maintain long-term stability due to the possible failure of catalytic sites. Herein, a novel dynamic electrocatalytic strategy with the liquid metal (i.e., gallium-tin, EGaSn) to facilitate LiPSs redox reaction is repor...