Nature Communications
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2022
·Vol. 13
·期 1
·1-12
·
IF 17.694
Cao Deqing,Tan Chuan,Chen Yuhui
Lithium carbonate plays a critical role in both lithium-carbon dioxide and lithium-air batteries as the main discharge product and a product of side reactions, respectively. Understanding the decomposition of lithium carbonate during electrochemical oxidation (during battery charging) is key for improving both chemistries, but the decomposition mechanisms and the role of the carbon substrate remain under debate. Here, we use an in-situ differential electrochemical mass spectrometry-gas chromatography coupling system to quantify the gas evolution during the electrochemical oxidation of lithium carbonate on carbon substrates. Our results show that lithium carbonate decomposes to carbon dioxide and singlet oxygen mainly via an electrochemical process instead of via a chemical process in an electrolyte of lithium bis(trifluoromethanesulfonyl)imide in tetraglyme. Singlet oxygen attacks the carbon substrate and electrolyte to form both carbon dioxide and carbon monoxide—approximately 20% of the net gas evolved originates from these side reactions. Additionally, we show that cobalt(II,III) oxide, a typical oxygen evolution catalyst, stabilizes the precursor of singlet oxygen, thus inhibiting the formation of singlet oxygen and consequent side reactions.
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Nature Communications
·
2022
·Vol. 13
·期 1
·1-12
·
IF 17.694
Zhang Zeyu,Sun Qingde,Lu Yue,Lu Feng,Mu Xulin,Wei Su-Huai,Sui Manling
Development of lead-free inorganic perovskite material, such as Cs 2 AgBiBr 6 , is of great importance to solve the toxicity and stability issues of traditional lead halide perovskite solar cells. However, due to a wide bandgap of Cs 2 AgBiBr 6 film, its light absorption ability is largely limited and the photoelectronic conversion efficiency is normally lower than 4.23%. In this text, by using a hydrogenation method, the bandgap of Cs 2 AgBiBr 6 films could be tunable from 2.18 eV to 1.64 eV. At the same time, the highest photoelectric conversion efficiency of hydrogenated Cs 2 AgBiBr 6 perovskite solar cell has been improved up to 6.37% with good environmental stability. Further investigations confirmed that the interstitial doping of atomic hydrogen in Cs 2 AgBiBr 6 lattice could not only adjust its valence and conduction band energy levels, but also optimize the carrier mobility and carrier lifetime. All these works provide an insightful strategy to fabricate high performance lead-free inorganic perovskite solar cells.
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Nature Communications
·
2022
·Vol. 13
·期 1
·1-10
·
IF 17.694
Zhou Wanlin,Su Hui,Cheng Weiren,Li Yuanli,Jiang Jingjing,Liu Meihuan,Yu Feifan,Wang Wei,Wei Shiqiang,Liu Qinghua
The electrochemical oxygen reduction reaction (ORR) is at the heart of modern sustainable energy technologies. However, the linear scaling relationship of this multistep reaction now becomes the bottleneck for accelerating kinetics. Herein, we propose a strategy of using intermetallic-distance-regulated atomic-scale bimetal assembly (ABA) that can catalyse direct O‒O radical breakage without the formation of redundant *OOH intermediates, which could regulate the inherent linear scaling relationship and cause the ORR on ABA to follow a fast-kinetic dual-sites mechanism. Using in situ synchrotron spectroscopy, we directly observe that a self-adjustable N-bridged Pt = N 2 = Fe assembly promotes the generation of a key intermediate state (Pt‒O‒O‒Fe) during the ORR process, resulting in high reaction kinetics and selectivity. The well-designed Pt = N 2 = Fe ABA catalyst achieves a nearly two orders of magnitude enhanced kinetic current density at the half-wave potential of 0.95 V relative to commercial Pt/C and an almost 99% efficiency of 4-electron pathway selectivity, making it one of the potential ORR catalysts for application to the energy device of zinc‒air cells. This study provides a helpful design principle for developing and optimizing other efficient ORR electrocatalysts.
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Nature Communications
·
2022
·Vol. 13
·期 1
·1-12
·
IF 17.694
Zhang Shuoqing,Li Ruhong,Hu Nan,Deng Tao,Weng Suting,Wu Zunchun,Lu Di,Zhang Haikuo,Zhang Junbo,Wang Xuefeng,Chen Lixin,Fan Liwu,Fan Xiulin
Electrolyte engineering advances Li metal batteries (LMBs) with high Coulombic efficiency (CE) by constructing LiF-rich solid electrolyte interphase (SEI). However, the low conductivity of LiF disturbs Li + diffusion across SEI, thus inducing Li + transfer-driven dendritic deposition. In this work, we establish a mechanistic model to decipher how the SEI affects Li plating in high-fluorine electrolytes. The presented theory depicts a linear correlation between the capacity loss and current density to identify the slope k (determined by Li + mobility of SEI components) as an indicator for describing the homogeneity of Li + flux across SEI, while the intercept dictates the maximum CE that electrolytes can achieve. This model inspires the design of an efficient electrolyte that generates dual-halide SEI to homogenize Li + distribution and Li deposition. The model-driven protocol offers a promising energetic analysis to evaluate the compatibility of electrolytes to Li anode, thus guiding the design of promising electrolytes for LMBs.
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Nature Communications
·
2022
·Vol. 13
·期 1
·1-17
·
IF 17.694
Guan Xin,Sun Liping,Shen Yuting,Jin Fengshan,Bo Xiaowan,Zhu Chunyan,Han Xiaoxia,Li Xiaolong,Chen Yu,Xu Huixiong,Yue Wenwen
Cancer recurrence after surgical resection (SR) is a considerable challenge, and the biological effect of SR on the tumor microenvironment (TME) that is pivotal in determining postsurgical treatment efficacy remains poorly understood. Here, with an experimental model, we demonstrate that the genomic landscape shaped by SR creates an immunosuppressive milieu characterized by hypoxia and high-influx of myeloid cells, fostering cancer progression and hindering PD-L1 blockade therapy. To address this issue, we engineer a radio-immunostimulant nanomedicine (IPI549@HMP) capable of targeting myeloid cells, and catalyzing endogenous H 2 O 2 into O 2 to achieve hypoxia-relieved radiotherapy (RT). The enhanced RT-mediated immunogenic effect results in postsurgical TME reprogramming and increased susceptibility to anti-PD-L1 therapy, which can suppress/eradicate locally residual and distant tumors, and elicits strong immune memory effects to resist tumor rechallenge. Our radioimmunotherapy points to a simple and effective therapeutic intervention against postsurgical cancer recurrence and metastasis.
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Nature Communications
·
2022
·Vol. 13
·期 1
·1-17
·
IF 17.694
Wang Weili,Zheng Huizhen,Jiang Jun,Li Zhi,Jiang Dongpeng,Shi Xiangru,Wang Hui,Jiang Jie,Xie Qianqian,Gao Meng,Chu Jianhong,Cai Xiaoming,Xia Tian,Li Ruibin
While hypoxia promotes carcinogenesis, tumour aggressiveness, metastasis, and resistance to oncological treatments, the impacts of hyperoxia on tumours are rarely explored because providing a long-lasting oxygen supply in vivo is a major challenge. Herein, we construct micro oxygen factories, namely, photosynthesis microcapsules (PMCs), by encapsulation of acquired cyanobacteria and upconversion nanoparticles in alginate microcapsules. This system enables a long-lasting oxygen supply through the conversion of external radiation into red-wavelength emissions for photosynthesis in cyanobacteria. PMC treatment suppresses the NF-kB pathway, HIF-1α production and cancer cell proliferation. Hyperoxic microenvironment created by an in vivo PMC implant inhibits hepatocarcinoma growth and metastasis and has synergistic effects together with anti-PD-1 in breast cancer. The engineering oxygen factories offer potential for tumour biology studies in hyperoxic microenvironments and inspire the exploration of oncological treatments.
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Advanced Fiber Materials
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2024
·
IF 17.2
Lan Boling,Zhong Cheng,Wang Shenglong,Ao Yong,Liu Yang,Sun Yue,Yang Tao,Tian Guo,Huang Longchao,Zhang Jieling,Deng Weili,Yang Weiqing
Respiration is a critical physiological process of the body and plays an essential role in maintaining human health. Wearable piezoelectric nanofiber-based respiratory monitoring has attracted much attention due to its self-power, high linearity, noninvasiveness, and convenience. However, the limited sensitivity of conventional piezoelectric nanofibers makes it difficult to meet medical and daily respiratory monitoring requirements due to their low electromechanical conversion efficiency. Here, we present a universally applicable, highly sensitive piezoelectric nanofiber characterized by a coaxial composite structure of polyvinylidene fluoride (PVDF) and carbon nanotube (CNT), which is denoted as PS-CC. Based on elucidating the enhancement mechanism from the percolation effect, PS-CC exhibits excellent sensing performance with a high sensitivity of 3.7 V/N and a fast response time of 20 ms for electromechanical conversion. As a proof-of-concept, the nanofiber membrane is seamlessly integrated into a facial mask, facilitating accurate recognition of respiratory states. With the assistance of a one-dimensional convolutional neural network (CNN), a PS-CC-based smart mask can recognize respiratory tracts and multiple breathing patterns with a classification accuracy of up to 97.8%. Notably, this work provides an effective strategy for monitoring respiratory diseases and offers widespread utility for daily health monitoring and clinical applications. Graphical abstract
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Nature Communications
·
2024
·Vol. 15
·期 1
·1-9
·
IF 14.7
Chen Ze,Wang Tairan,Wu Zhuoxi,Hou Yue,Chen Ao,Wang Yanbo,Huang Zhaodong,Schmidt Oliver G.,Zhu Minshen,Fan Jun,Zhi Chunyi
The high redox potential of Zn 0/2+ leads to low voltage of Zn batteries and therefore low energy density, plaguing deployment of Zn batteries in many energy-demanding applications. Though employing high-voltage cathode like spinel LiNi 0.5 Mn 1.5 O 4 can increase the voltages of Zn batteries, Zn 2+ ions will be immobilized in LiNi 0.5 Mn 1.5 O 4 once intercalated, resulting in irreversibility. Here, we design a polymer hetero-electrolyte consisting of an anode layer with Zn 2+ ions as charge carriers and a cathode layer that blocks the Zn 2+ ion shuttle, which allows separated Zn and Li reversibility. As such, the Zn ‖ LNMO cell exhibits up to 2.4 V discharge voltage and 450 stable cycles with high reversible capacity, which are also attained in a scale-up pouch cell. The pouch cell shows a low self-discharge after resting for 28 days. The designed electrolyte paves the way to develop high-voltage Zn batteries based on reversible lithiated cathodes.
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MICROCHIMICA ACTA
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2025
·Vol. 192
·期 4
·1-11
·
IF 5.3
Mei Lin,Wei Bingjie,Liu Chunyan,Zhao Mengting,Cui Tian,Wei Xiangyang
A highly efficient colorimetric sensor was developed for detecting glutathione using polyvinylpyrrolidone-stabilized ultra-small Fe 3 O 4 nanoparticles integrated with graphene oxide (GO-Fe 3 O 4 ). These nanoparticles are highly water-dispersible and uniformly distributed, enabling extensive interaction with the analyte and enhancing detection sensitivity. The integration of Fe 3 O 4 nanoparticles on the graphene oxide surface prevents aggregation and exposes more active sites, thereby enhancing their catalytic activity significantly. The GO-Fe 3 O 4 nanocomposites exhibit a dramatically enhanced Fenton reaction, showing a fourfold increase in catalytic effect compared to bare Fe 3 O 4 nanoparticles. This is attributed to the synergistic peroxidase-like activity within the 3,3′,5,5′-tetramethylbenzidine (TMB)-hydrogen peroxide colorimetric system. Moreover, the GO-Fe 3 O 4 nanozyme has an excellent binding affinity to TMB, which is up to tenfold higher than that of horseradish peroxidase. The TMB is catalyzed by the GO-Fe 3 O 4 nanozyme to produce a blue oxidized form, and the presence of glutathione selectively inhibits this color change. This inhibition forms the basis for the quantitative determination of glutathione. Under optimal conditions, the colorimetric sensor demonstrated a linear response to glutathione concentrations ranging from 0.1 to 10 μmol/L, with a detection limit as low as 9.17 nmol/L ( S/N = 3). The developed method showcased excellent selectivity, reproducibility, and accuracy. It was effectively used to determine glutathione in rat serum samples and monitor its pharmacokinetics in vivo. Graphical
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Nature Communications
·
2024
·Vol. 15
·期 1
·1-10
·
IF 14.7
Pan Xin,Zhuang Yixi,He Wei,Lin Cunjian,Mei Lefu,Chen Changjian,Xue Hao,Sun Zhigang,Wang Chunfeng,Peng Dengfeng,Zheng Yanqing,Pan Caofeng,Wang Lixin,Xie Rong-Jun
Mechanoluminescence (ML) sensing technologies open up new opportunities for intelligent sensors, self-powered displays and wearable devices. However, the emission efficiency of ML materials reported so far still fails to meet the growing application requirements due to the insufficiently understood mechano-to-photon conversion mechanism. Herein, we propose to quantify the ability of different phases to gain or lose electrons under friction (defined as triboelectric series), and reveal that the inorganic-organic interfacial triboelectricity is a key factor in determining the ML in inorganic-organic composites. A positive correlation between the difference in triboelectric series and the ML intensity is established in a series of composites, and a 20-fold increase in ML intensity is finally obtained by selecting an appropriate inorganic-organic combination. The interfacial triboelectricity-regulated ML is further demonstrated in multi-interface systems that include an inorganic phosphor-organic matrix and organic matrix-force applicator interfaces, and again confirmed by self-oxidization and reduction of emission centers under continuous mechanical stimulus. This work not only gives direct experimental evidences for the underlying mechanism of ML, but also provides guidelines for rationally designing high-efficiency ML materials.
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MICROCHIMICA ACTA
·
2025
·Vol. 192
·期 4
·1-13
·
IF 5.3
Li Yang,Long Feng,Han Shitong,Wang Yi,Zhu Anna
Timely and accurate detection of the virus is of great significance to prevent the virus’s harm and control the epidemic. Here, an aptasensor based on the principle of promoting hybridization through aptamer conformational change was designed to quantitatively detect the spike (S) protein of SARS-CoV-2. When the S protein binds to the 3' end of the aptamer, the 5' end of the aptamer tansforms into a straight hybridization region, which will greatly facilitate the hybridization with complementary DNA (cDNA). In the absence of S protein, hybridization is less likely to occur due to the complex G-quadruplex structure of aptamer. According to this principle, cDNA is modified onto magnetic beads (MBs) or onto the optical fiber probe of an evanescent wave fluorescence aptasensor (EWFA) detection platform to capture the fluorescently labeled aptamer-S protein conjugate, two kinds of quantitative detection methods for SARS-CoV-2 S protein were established. In particular, simple, rapid and sensitive detection could be obtained based on the EWFA detection platform, in which the whole detection procedure including the measurement and regeneration takes only 14 min, the LOD is 5.34 ng/mL, the linear response range is 141.49 to 9507.36 ng/mL, and the optical fiber probe could be reused for 19 times. The EWFA detection platform is also potentially applicable to detect other protein biomarkers only by replacing the specifically modified optical fiber probes. Graphical
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Journal of Sustainable Metallurgy
·
2024
·Vol. 10
·期 2
·893-902
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IF 2.5
You Conglin,Li Dongdong,Fan Yanfei,Gao Dandan,Han Li,Zeng Dewen
Lithium aluminum layered double hydroxide chlorides (LADH-Cl) are the only industrial-level lithium sorbents. However, as an applied material, the composition-structure-property-performance relation is far from well constrained, leaving the manufacture and application of LADH-Cl lithium sorbents empirical rather than rational. Herein, we studied the phase evolution of gibbsite phase Al(OH) 3 in concentrated LiOH aqueous solution, suggesting the formation of lithiated lithium aluminum layered double hydroxide (LADH-OH) with Al:Li molar ratio 2. However, LADH-OH is not an active ingredient as a lithium sorbent. The neutralization of LADH-OH with a dilute HCl aqueous solution resulted in the formation of the active LADH-Cl phase. Unlike the traditional LADH-Cl phase (g-LADH-Cl) generated from direct LiCl intercalation of gibbsite, LADH-OH derived LADH-Cl (b-LADH-Cl) has a topological parent of bayerite instead of gibbsite. This is one of the most important roots for different performances. Another source for the different performance is very likely from variations of the particle size and morphology when the raw gibbsite reacted with LiCl or LiOH aqueous solution. Nevertheless, we found that the limiting-delithiation of b-LADH-Cl is still the same as g-LADH-Cl, that is only maximum 1/3 lithium can be delithiated from the LADH-Cl phase without any decomposition into gibbsite or bayerite. This concluded that b-LADH-Cl and g-LADH-Cl have the same reversible lithium “sorption–desorption” capacity, even through different lithium affinity and sorption kinetics. Also, notably, the “sorption–desorption” performance of the optimal sorbent is very sensitive to the properties of service brines. These results substantially enlarged our knowledge of the LADH-Cl phase and provided a demo of the rational manufacture of lithium sorbent. Graphical Abstract
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