Abstract:Zinc metal anode in aqueous zinc-ion batteries (AZIBs) is considerably impeded by uncontrollable dendrite growth and intricately water-induced corrosion, leading to low Coulombic efficiency (CE) and limited lifespan. Herein, a...
“…[ 58–61 ] And the negative surface charges can lead to the closely adhesion between zinc anode and CG separator under the electrostatic attraction and strong binding energy between O groups and zinc anode (OH/Zn: −7.64 eV, O/Zn: −26.33 eV), [ 62 ] which greatly shortens the path of Zn 2+ ions transmission and constructs a special separator–anode interface. [ 62,63 ] Additionally, the negative charged CG separator surface can effectively deanion (SO 4 2– ) via the electrostatic repulsion, [ 64 ] thus suppressing the formation of side effects (Zn 4 SO 4 (OH) 6 ·5H 2 O), which is demonstrated in Figure S7d, Supporting Information. Furthermore, the electrochemical impedance spectrum (EIS) proves that the fast ion diffusion and quick charge transfer process can be achieved by CG separator (Figure 3d).…”
The dendrite issues associated with zinc anode lead to safety hazards and sluggish reaction kinetics, and largely restrain widespread application of aqueous zinc ion batteries (ZIBs). Herein, a functional separator composed of cellulose nanofibers and graphene oxide (CG) is developed for dendrite‐free and exceptionally stable ZIBs, realized by uniform hexagonal zinc deposits with manipulated crystallographic orientation (002) plane. This CG separator with negative surface charges and abundant zincophilic‐O groups ensures the strong interaction between the separator and zinc species, simultaneously inducing Zn(002) deposition due to the low mismatch between (002)Zn and (002)GO, thus initiating the preferential orientation of the zinc growth along the horizontal direction due to strong Zn binding ability, and uniform interfacial charge of Zn(002) deposition. Furthermore, the CG separator can effectively promote the uniform nucleation of Zn2+ and eliminate side effects. Accordingly, extremely low polarization of 58 mV at 0.5 mA cm−2, and ultralong cycle life over 1750 h at 2 mA cm−2 and 400 h at 20 mA cm−2 are achieved for the zinc anode. Notably, the CG separator significantly boosts rate capability and cyclability of coin‐type full batteries (Zn||Zn(CF3SO3)2||V2O5, Zn||ZnSO4+MnSO4||MnO2/graphite) and a flexible soft‐packaged battery (Zn||MnO2). Therefore, this work introduces a sustainability consideration in to the design of separators for constructing dendrite‐free ZIBs.
“…[ 58–61 ] And the negative surface charges can lead to the closely adhesion between zinc anode and CG separator under the electrostatic attraction and strong binding energy between O groups and zinc anode (OH/Zn: −7.64 eV, O/Zn: −26.33 eV), [ 62 ] which greatly shortens the path of Zn 2+ ions transmission and constructs a special separator–anode interface. [ 62,63 ] Additionally, the negative charged CG separator surface can effectively deanion (SO 4 2– ) via the electrostatic repulsion, [ 64 ] thus suppressing the formation of side effects (Zn 4 SO 4 (OH) 6 ·5H 2 O), which is demonstrated in Figure S7d, Supporting Information. Furthermore, the electrochemical impedance spectrum (EIS) proves that the fast ion diffusion and quick charge transfer process can be achieved by CG separator (Figure 3d).…”
The dendrite issues associated with zinc anode lead to safety hazards and sluggish reaction kinetics, and largely restrain widespread application of aqueous zinc ion batteries (ZIBs). Herein, a functional separator composed of cellulose nanofibers and graphene oxide (CG) is developed for dendrite‐free and exceptionally stable ZIBs, realized by uniform hexagonal zinc deposits with manipulated crystallographic orientation (002) plane. This CG separator with negative surface charges and abundant zincophilic‐O groups ensures the strong interaction between the separator and zinc species, simultaneously inducing Zn(002) deposition due to the low mismatch between (002)Zn and (002)GO, thus initiating the preferential orientation of the zinc growth along the horizontal direction due to strong Zn binding ability, and uniform interfacial charge of Zn(002) deposition. Furthermore, the CG separator can effectively promote the uniform nucleation of Zn2+ and eliminate side effects. Accordingly, extremely low polarization of 58 mV at 0.5 mA cm−2, and ultralong cycle life over 1750 h at 2 mA cm−2 and 400 h at 20 mA cm−2 are achieved for the zinc anode. Notably, the CG separator significantly boosts rate capability and cyclability of coin‐type full batteries (Zn||Zn(CF3SO3)2||V2O5, Zn||ZnSO4+MnSO4||MnO2/graphite) and a flexible soft‐packaged battery (Zn||MnO2). Therefore, this work introduces a sustainability consideration in to the design of separators for constructing dendrite‐free ZIBs.
“…The work demonstrated that the CNC–graphene interface layer with negative surface charges could simultaneously generate a deanionization shock by spreading cations but screening anions to obtain redirected Zn deposition parallel to the (0002) Zn plane. [ 38 ] To sum up, the development of nanocellulose for EES has received wide attention due to the advantages of its intrinsic properties and structures, as demonstrated in Figure 4.…”
Section: Preparation and Properties Of Nanocellulosementioning
With the increasing demand for wearable electronics (such as smartwatch equipment, wearable health monitoring systems, and human–robot interface units), flexible energy storage systems with eco‐friendly, low‐cost, multifunctional characteristics, and high electrochemical performances are imperative to be constructed. Nanocellulose with sustainable natural abundance, superb properties, and unique structures has emerged as a promising nanomaterial, which shows significant potential for fabricating functional energy storage systems. This review is intended to provide novel perspectives on the combination of nanocellulose with other electrochemical materials to design and fabricate nanocellulose‐based flexible composites for advanced energy storage devices. First, the unique structural characteristics and properties of nanocellulose are briefly introduced. Second, the structure–property–application relationships of these composites are addressed to optimize their performances from the perspective of processing technologies and micro/nano‐interface structure. Next, the recent specific applications of nanocellulose‐based composites, ranging from flexible lithium‐ion batteries and electrochemical supercapacitors to emerging electrochemical energy storage devices, such as lithium‐sulfur batteries, sodium‐ion batteries, and zinc‐ion batteries, are comprehensively discussed. Finally, the current challenges and future developments in nanocellulose‐based composites for the next generation of flexible energy storage systems are proposed.
“…Zn anode surface modifications (such as ZrO 2 and graphene) can guide the even charge distribution and contribute to the controllable nucleation sites for Zn 2+ , which significantly suppressed dendrites growth in repeated cycling. [17,[24][25][26][27] The electrolyte-based approaches positively influence the performance of Zn anode by forming an artificial solid electrolyte interface on Zn anode surface or decreasing the activeness of H 2 O in the electrolyte, leading to the dendrite-free anode. [28][29][30][31] However, these two methods usually increase the internal impedance or polarization.…”
The detrimental hydrogen evolution side reaction is one of the major issues hindering the commercialization of Zn metal anode in high-safety and lowcost rechargeable aqueous batteries. Herein, the authors present a Sn alloying approach to effectively inhibit the hydrogen evolution and dendrite growth of the Zn metal anode. Through in situ monitoring of the hydrogen production during repeated plating/stripping tests, it is quantitatively demonstrated that the hydrogen evolution of alloy electrode with appropriate Sn amount is only half of that of pure Zn electrode. Furthermore, the Sn alloying allows for favorable Zn nucleation sites, lowering the Zn nucleation energy barrier and promoting more uniform Zn deposition. The Zn-Sn alloy electrode offers muchimproved plating/stripping cycling, that is, over 240 h at 5 mA cm −2 and 35.2% depth of discharge. This work provides a practically viable strategy to stabilize Zn metal electrode in rechargeable aqueous batteries.
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