Abstract
Uncontrollable dendrite growth is closely related to non‐uniform reaction environments. However, there is a lack of understanding and analysis methods to probe the localized electrochemical ...environment (LEE). Here the effects of the LEE are investigated, including localized ion concentrations, current density, and electric potential, on metal plating/stripping dynamics and dendrite minimization. A novel in situ 3D microscopy technique is developed to image the morphology dynamics and deposition rate of Zn plating/stripping processes on 3D Zn–Mn anodes. Using the in situ 3D microscope, the electrode morphology changes during the reactions are directly imaged and Zn deposition rate maps at different time points are obtained. It is found that reaction kinetics are highly correlated to LEE and electrode morphology. To further quantify the LEE effects, the digital twin technique is employed that allows the accurate calculation of the electrochemical environments, such as localized ion concentrations, current density, and electric potential, which cannot be directly measured from experiments. It is found that the curvature of the 3D electrode surface determines the LEE and significantly influences reaction kinetics. This provides a new strategy to minimize the dendrite formation by designing and optimizing the 3D geometry of the electrode to control the LEE.
Abstract
Uncontrollable dendrite growth is closely related to non‐uniform reaction environments. However, there is a lack of understanding and analysis methods to probe the localized electrochemical ...environment (LEE). Here the effects of the LEE are investigated, including localized ion concentrations, current density, and electric potential, on metal plating/stripping dynamics and dendrite minimization. A novel in situ 3D microscopy technique is developed to image the morphology dynamics and deposition rate of Zn plating/stripping processes on 3D Zn–Mn anodes. Using the in situ 3D microscope, the electrode morphology changes during the reactions are directly imaged and Zn deposition rate maps at different time points are obtained. It is found that reaction kinetics are highly correlated to LEE and electrode morphology. To further quantify the LEE effects, the digital twin technique is employed that allows the accurate calculation of the electrochemical environments, such as localized ion concentrations, current density, and electric potential, which cannot be directly measured from experiments. It is found that the curvature of the 3D electrode surface determines the LEE and significantly influences reaction kinetics. This provides a new strategy to minimize the dendrite formation by designing and optimizing the 3D geometry of the electrode to control the LEE.
Protein‐bound uremic toxins (PBUTs) accumulate at high plasma levels and cause various deleterious effects in end‐stage renal disease patients because their removal by conventional hemodialysis is ...severely limited by their low free‐fraction levels in plasma. Here, we assessed the extent to which solute removal can be increased by adding liposomes to the dialysate. The uptake of liposomes by direct incubation in vitro showed an obvious dose‐response relationship for p‐cresyl sulfate (PCS) and indoxyl sulfate (IS) but not for hippuric acid (HA). The percent removal of both PCS and IS but not of HA was gradually increased with the increased concentration of liposomes in a rapid equilibrium dialysis setup. In vitro closed circulation showed that adding liposomes to the dialysate markedly increased the dialysances of PBUTs without greatly altering that of urea and creatinine. In vivo experiments in uremic rats demonstrated that adding liposomes to the dialysate resulted in higher reduction ratios (RRs) and more total solute removal (TSR) for several PBUTs compared to the conventional dialysate, which was approximately similar to the addition of bovine serum albumin to the dialysate. These findings highlight that as an adjunct to conventional hemodialysis, addition of liposomes to the dialysate could significantly improve the removal of protein‐bound uremic solutes without greatly altering the removal of small, water‐soluble solutes.
Background
Protein-bound uremic toxins (PBUTs) are poorly cleared by peritoneal dialysis (PD). This study aimed to enhance PBUT removal in PD by adding a binder to the peritoneal dialysate and to ...evaluate the feasibility and efficacy of liposome-supported PD (LSPD) to increase the removal of PBUTs compared with albumin PD.
Methods
Removal of p-cresyl sulfate (PCS), indoxyl sulfate (IS), and indole-3-acetic acid (3-IAA) was first evaluated in an in vitro PD model using artificial plasma preloaded with test solutes. Male Sprague-Dawley rats (n = 24) were then subjected to 5/6 nephrectomy and fed for 16 weeks to establish end-stage renal failure, after which they were treated with either conventional glucose-based PD, albumin-based PD, or liposome-based PD. Removal of PBUTs and small water-soluble solutes was determined during a 6-hour PD dwell.
Results
In vitro experiments showed that adding albumin as a toxin binder to the dialysate markedly increased the removal of PCS, IS, and 3-IAA compared with the control. The uptake capacity of liposomes was comparable with that of albumin for PCS and 3-IAA, though slightly inferior for IS. In vivo PD in uremic rats demonstrated that LSPD resulted in higher intraperitoneal concentrations and more total mass removal for PBUTs than the conventional glucose-based PD, which was comparable with albumin PD.
Conclusions
Supplementing conventional glucose-based PD solutions with a binder could efficiently increase the removal of PBUTs. This preliminary study suggested that LSPD may be a promising alternative to albumin PD for increasing PBUT removal in the development of next-generation PD solutions for PD patients.
Tin (Sn)-based materials are one of most promising candidates for rechargeable (Li+ and Na+ ion) batteries because of their high theoretical capacities (993 mAh/g for Li4.4Sn and 847 mAh/g for ...Na15Sn4) and reasonable working potentials. However, Sn-based anodes suffer from huge volume changes during cycling that hinder the applications in commercialized rechargeable batteries. Unique particle engineering to fabricate Sncore–carbonshell (Sn@C) particles has been shown to address or circumvent these problems. In this work, a distinct core–shell-structured Sn@C anode material has been successfully developed by using a one-step and template-free process (colloidal spray pyrolysis). A comprehensive analysis of chemical reaction kinetics of core–shell particles assists the product design to control the particle composition and structure by tuning the process variables, such as reaction temperature and cosolvent concentration. The unique Sn@C anode delivers a high capacity of 720 mAh/g after 300 cycles at 0.5C for lithium-ion batteries and a high capacity of >500 mAh/g at 0.2C for sodium-ion batteries. More importantly, this work advances the design of high-performance Sn@C composites for lithium/sodium-ion batteries in scalable process development, particle engineering, and material innovation.
The effect of Mg2+ ions substituted into the anatase lattice on the charge recombination and band-edge movement in dye-sensitized solar cells was investigated in this study. The HRTEM results ...indicated that Mg2+ ions incorporation into the TiO2 lattice led to the increased lattice spacing of the (101) plane of the anatase phase. Mg2+-doped TiO2 could produce a blue shift in the optical absorption edge compared with that of the untreated samples. Detailed analysis of the open-circuit photovoltage (V oc) under different surface charge densities showed that the Mg2+-doped TiO2 samples resulted in the negative shift of the TiO2 conduction band about 70 mV in comparison with the untreated samples. From Raman spectra and light intensity-dependent variation of the short-circuit current density (J sc) of the solar cells, it could be concluded that the decreased efficiency of electron injection for DSCs with Mg2+-doped TiO2 was attributed to the negative shift of the band edge in the Mg2+-doped TiO2 electrode to obtain a decreased J sc. The electron diffusion coefficient in Mg2+-doped TiO2 was found to be higher than that in TiO2 at the same photoelectron density. We present evidence that the increase of trap states in Mg2+-doped TiO2 as recombination channels to decrease the electron lifetime could compensate for the effect of band-gap widening to obtain a slightly increased V oc for DSCs with Mg2+-doped TiO2. It is suggested that the recombination channels should be suppressed to enhance the performance of dye-sensitized Mg2+-doped TiO2 solar cells.
Artificial liver support systems (ALSS), represented by albumin dialysis, are designed to replace the liver detoxification function and to serve as supportive therapy until liver transplantation or ...liver regeneration. We introduce liposome, which is majorly formed by soybean lecithin as the adsorbent nanomaterial in dialysate for the removal of protein-bound and liver failure-related solutes. The binding rate was detected by ultrafiltration column. In vitro and in vivo dialysis was performed in a recirculation system. Unconjugated bilirubin (52.83-99.87%) and bile salts (50.54-94.75%) were bound by liposomes (5-80 g/L) in a dose-response relationship. The in vitro haemodialysis model showed that the concentration of unconjugated bilirubin (45.64 ± 0.90 μmol/L vs. 54.47 ± 3.48 μmol/L, p < 0.05) and bile salts (153.75 ± 7.72 μmol/L vs. 180.72 ± 7.95 μmol/L, p < 0.05) were significantly decreased in the liposome dialysis group than in the phosphate buffer saline group. The in vivo haemodialysis model showed that 40 g/L liposome-containing dialysate led to a significant higher reduction ratio in total bilirubin (6.56 ± 5.72% vs. −1.86 ± 5.99%, p < 0.05) and more total bile acids (7.63 ± 5.27 μmol vs. 2.13 ± 2.32 μmol, p < 0.05) extracted in the dialysate in comparison with the conventional dialysate. In conclusion, the liposome-added dialysate proved to impose good extraction effects on the unconjugated bilirubin and bile salts. These findings indicate that conventional dialysate supported by this nanomaterial can markedly improve the removal of protein-bound and liver failure-related solutes, thus suggesting a novel and promising liver dialysis system.
While trying to optimize the dialysis clearances of protein-bound uremic toxins (PBUTs), their percentage protein binding (% PB) is an important parameter. We evaluated the effects of ionic strength, ...pH change and chemical displacers on the dissociation of PBUTs from albumin in vitro.
PBUTs, such as 3-Carboxy-4-methyl-5-propyl-2-furan-propanoic acid (CMPF), p-cresylsulfate (PCS), indoxyl sulfate (IS) and indole-3-acetic acid (IAA), were spiked with human serum albumin (HSA) solution prepared with different Nacl concentrations and pH values or in the presence of a series of chemical displacers. Ultrafiltration was performed to separate the free and bound fractions, and the % PB of each PBUT was calculated.
For all 4 compounds, their % PB decreased with increasing ionic strength, while only slight changes occurred when the pH of the test solution increased from pH 6.0 to pH 8.5; PCS, IS and 3-IAA were relatively easily dissociated from albumin by drug displacement, while CMPF was released from HSA by all studied drugs with difficulty; the PB % for CMPF, PCS, IS and 3-IAA decreased most remarkably in the presence of free fatty acids, such as oleic acid (41.73% for CMPF, 29.9% for PCS, 23.22% for IS, and 20.34% for 3-IAA) and linoleic acid (43.12% for CMPF, 16.65% for PCS, 29.99% for IS, and 16.29% for 3-IAA).
The protein binding of PBUTs can be decreased by higher ionic strength, increased pH and the presence of some chemical displacers, including free fatty acids. Effective dialytic removal of PBUTs may be achieved by applying these methods jointly to blood-purification techniques.
Recycling lithium from spent batteries is challenging because of problems with poor purity and contamination. Here, we propose a green and sustainable lithium recovery strategy for spent batteries ...containing LiFePO
4
, LiCoO
2
, and LiNi
0.5
Co
0.2
Mn
0.3
O
2
electrodes. Our proposed configuration of “lithium-rich electrode || LLZTO@LiTFSI+P3HT || LiOH” system achieves double-side and roll-to-roll recycling of lithium-containing electrode without destroying its integrity. The LiTFSI+P3HT-modified LLZTO membrane also solves the H
+
/Li
+
exchange problem and realizes a waterproof protection of bare LLZTO in the aqueous working environment. On the basis of these advantages, our system shows high Li selectivity (97%) and excellent Faradaic efficiency (≥97%), achieving high-purity (99%) LiOH along with the production of H
2
. The Li extraction processes for spent LiFePO
4
, LiNi
0.5
Co
0.2
Mn
0.3
O
2
, and LiCoO
2
batteries is shown to be economically feasible. Therefore, this study provides a previously unexplored technology with low energy consumption as well as high economic and environmental benefits to realize sustainable lithium recycling from spent batteries.
The P3HT-modified LLZTO ceramic electrolyte enables high-purity lithium recycling from various spent batteries.
