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INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES · 2020 ·Vol. 21 ·期 11 ·3939 · IF 4.556

A Microarray Screening Platform with an Experimental Conditions Gradient Generator for the High-Throughput Synthesis of Micro/Nanosized Calcium Phosphates

Xiaoyu Li,Zhifeng Shi,Lei Liu,Guanglin Zhu,Jianhua Zhou,Xuetao Shi,Yingjun Wang

Calcium phosphates (CaP) represent an impressive kind of biomedical material due to their excellent biocompatibility, bioactivity, and biodegradability. Their morphology and structure highly influence their properties and applications. Whilst great progress has been made in research on biomedical materials, there is still a need to develop a method that can rapidly synthesize and screen micro/nanosized biomedical materials. Here, we utilized a microarray screening platform that could provide the high-throughput synthesis of biomedical materials and screen the vital reaction conditions. With this screening platform, 9 × 9 sets of parallel experiments could be conducted simultaneously with one- or two-dimensions of key reaction condition gradients. We used this platform to establish a one-dimensional gradient of the pH and citrate concentration and a two-dimensional gradient of both the Ca/P ratio and pH to synthesize CaP particles with various morphologies. This screening platform also shows the potential to be extended to other reaction systems for rapid high-throughput screening.Keywords:microfluidics;high-throughput;concentration gradient;calcium phosphates

CAS / MDL: 1310-73-2
研究领域: 材料科学 · 生物医学工程
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Materials Chemistry Frontiers · 2025 · IF 6.4

Capillary force and concentration gradient promote bioprocessing-inspired formation of ultralong fluorapatite nanorods under confinement

Yonglang Yu,Ping Yuan,Zhengyi Fu,Zhaoyong Zou

Crystallization within small volumes rather than bulk solutions is a common phenomenon found during materials synthesis and biomineralization processes. However, the driving forces for mass transport and crystallization under confined environment remain elusive. Here, inspired by the intrafibrillar collagen mineralization process, we investigate the infiltration and crystallization mechanisms of fluorapatite (FAP) within confined channels by comparing anodic aluminum oxide and track-etched template with different surface properties. The results demonstrate that, similar to intrafibrillar collagen mineralization, the capillary force, along with specific interaction between confined channel surface and mineral precursors, is the main driving force for initial infiltration of liquid precursors into confined channels, leading to the nucleation FAP nanocrystals on the surface of channels. We elucidate the critical role of negatively charged polyacrylic acid in promoting the formation liquid precursors for successful infiltration into confined channels and controlling the crystallization kinetics within channels. The formation of FAP nanorods proceed by further promoting the ion diffusion via a concentration gradient resulted from the lower local concentration surrounding FAP crystals. Furthermore, FAP nanocrystals exhibit progressive alignment along the channel direction during subsequent crystal growth stage and ultralong FAP nanorods with a length of more than 25 μm could be obtained. The collective findings underscore the pivotal role of the structure and surface properties of nanoscale confined environment in controlling the infiltration and crystallization pathways of inorganic crystals and establish a foundation for controlled synthesis of biomimetic materials under confinement.

CAS / MDL: 9003-01-4
研究领域: 材料科学 · 生物矿化 · 仿生合成
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Symmetry-Basel · 2025 ·Vol. 17 ·期 6 ·826 · IF 2.2

Flexible Concentration Gradient Droplet Generation via Partitioning–Recombination in a Shear Flow-Driven Multilayer Microfluidic Chip

Linkai Yu,Qingyang Feng,Yifan Chen,Yongji Wu,Haizhen Sun,Hao Yang,Lining Sun

Concentration gradient generation plays a pivotal role in advancing applications across drug screening, chemical synthesis, and biomolecular studies, yet conventional methods remain constrained by labor-intensive workflows, limited throughput, and inflexible gradient control. This study presents a novel multilayer microfluidic chip leveraging shear flow-driven partitioning–recombination mechanisms to enable the flexible and high-throughput generation of concentration gradient droplets. The chip integrates interactive upper and lower polydimethylsiloxane (PDMS) layers, where sequential fluid distribution and recombination are achieved through circular and radial channels while shear forces from the oil phase induce droplet formation. Numerical simulations validated the dynamic pressure-driven concentration gradient formation, demonstrating linear gradient profiles across multiple outlets under varied flow conditions. The experimental results revealed that the shear flow mode significantly enhances mixing uniformity and droplet generation efficiency compared to continuous flow operations, attributed to intensified interfacial interactions within contraction–expansion serpentine channels. By modulating hydrodynamic parameters such as aqueous- and oil-phase flow rates, this system achieved tunable gradient slopes and droplet sizes, underscoring the intrinsic relationship between flow dynamics and gradient formation. The proposed device eliminates reliance on complex channel networks, offering a compact and scalable platform for parallelized gradient generation. This work provides a robust framework for optimizing microfluidic-based concentration gradient systems, with broad implications for high-throughput screening, combinatorial chemistry, and precision biomolecular assays.

CAS / MDL: 497-19-8 64-17-5
研究领域: 药物筛选 · 化学合成 · 生物分子研究
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY · 2023 · IF 4.5

Understanding natural convection in low-concentration electrochemical system: Validation of the convection modes

Biwu Cai,Jianbang Ge,Fei Zhu,Yang Gao,Shuqiang Jiao

Natural convection could arise under density gradients of solutions caused by the electrochemical reaction occurring on the electrode surface. This density-driven convection decays rapidly with the decreasing redox concentration, and becomes negligible in dilute solutions (1–2 mM). However, steady-state voltammetry is still observed in these dilute solutions due to the presence of a convection–diffusion layer. Here we studied natural convection effects in low-concentration (5–30 mM) redox solutions and clarified the convection modes in these transient-concentration solutions using cyclic voltammetry and chronoamperometry. The combined theoretical–experimental work demonstrated the coexistence of convection–diffusion layer and density-driven convection. With the use of a 150-μm-radius Pt microelectrode, the convection–diffusion layer convection dominated natural convection in dilute solution (1–5 mM), reinforced mass transport with density-driven convection in low redox concentrations (5–11 mM), and suppressed the density-driven convection at high redox concentrations (>15 mM). The zone diagrams delineating the transition from diffusion to convection were then established to reveal the effects of electrode radius, thickness of the convection–diffusion layer, time scale, and redox concentration on natural convection. Consequently, the use of microelectrodes (∼25 μm radius) could greatly inhibit natural convection effects in 30 mM redox solution.

CAS / MDL: 7447-40-7
研究领域: 电化学 · 传质工程 · 物理化学
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Journal of the American Chemical Society · 2024 · IF 14.4

Ion-Concentration-Hopping Heterolayer Gel for Ultrahigh Gradient Energy Conversion

Weipeng Chen,Ke Zhou,Zhixin Wu,Linsen Yang,Yahui Xie,Xue Meng,Ziguang Zhao,Liping Wen

Conventional solid ion channel systems relying on single one- or two-dimensional confined nanochannels enabled selective and ultrafast convective ion transport. However, due to intrinsic solid channel stacking, these systems often face pore–pore polarization and ion concentration blockage, thereby restricting their efficiency in macroscale ion transport. Here, we constructed a soft heterolayer-gel system that integrated an ion-selective hydrogel layer with a water-barrier organogel layer, achieving ultrahigh cation selectivity and flux and effectively providing high-efficiency gradient energy conversion on a macroscale order of magnitude. Specifically, the hydrogel layer featured an unconfined 3D network, where the fluctuations of highly hydrated polyelectrolyte chains driven by thermal dynamics enhanced cation selectivity and mitigated transfer energy barriers. Such chain fluctuation mechanisms facilitated ion-cluster internal transmission, thereby enhancing ion concentration hopping for more efficient ion-selective transport. Compared to the existing rigid nanochannel-based gradient energy conversion systems, such a heterogel-based power generator exhibited a record power density of 192.90 and 1.07 W/m2 at the square micrometer scale and square centimeter scale, respectively (under a 500-fold artificial solution). We anticipate that such heterolayer gels would be a promising candidate for energy separation and storage applications.

研究领域: 材料科学 · 能源工程 · 化学工程
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CHEMICAL ENGINEERING JOURNAL · 2024 · IF 13.3

Strong concentration gradient effect and weak solvation effect in thermopower enhancement in K3Fe(CN)6/ K4Fe(CN)6 aqueous electrolyte with ethanol addition

Shouze Li,Zhou Li,Dongyan Xu,Run Hu

Emerging thermocells exhibit a significant potential in low-grade heat harvesting owe to their high mV-scale thermopower, low cost, and high robustness. Fundamentally, three effects contribute to the thermopower enhancement of liquid thermocells, i.e. original concentration effect, solvation effect, and normalized concentration gradient effect. Yet, the contribution of the solvation effects and the normalized concentration gradient in organic solvents remains a subject of debate. In this paper, we integrate experiments, spectral analysis, and electrochemical theory to demonstrate that the normalized concentration gradient dominates the enhancement of thermopower in the investigated organic solvents, whereas the solvation effect is weak. Further, the introduction of ethanol results in a thermosensitive solubility of K 4 Fe(CN) 6 and a minimal concentration at the cold end, which establishes a huge substantial normalized Fe(CN) 6 4- concentration gradient and increases the Seebeck coefficient to 3.4 mV/K. Simultaneously, the precipitation resulting from the introduction of an organic solvent notably diminishes the heat convection within the system. As a result, the optimized TC-35EtOH system yields a ZT value (0.094) and Carnot-relative efficiency (2.52 %) that are 7 times greater than those of its initial counterpart. Additionally, the system’s high power density of 3.64 W/m 2 suggests its potential for harnessing low-grade heat waste energy.

研究领域: 物理化学 · 能源材料科学
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Materials Today · 2022 · IF 26.943

Diffusion-induced stress optimization by boosted surface Li-concentration for single-crystal Ni-rich layered cathodes

Yun Liu,Qi Wang,Lai Chen,Zhiming Xiao,Xinming Fan,Shuailing Ma,Lei Ming,Akhil Tayal,Bao Zhang,Feng Wu,Xing Ou

Nickel-rich layered LiNi x Co y Mn 1- x - y O 2 (NCM, x  ≥ 0.83) is considered as a promising cathode material for lithium-ion batteries (LIBs), owing to its satisfying specific energy. However, the undesired phase transformation from layered into rock-salt at the NCM surface will easily induce Li concentration gradient during cycling, which hinders the Li-ions diffusion and leads to the gradual accumulation of inner stress with the appearance of microcracks. Herein, we propose a surficial engineering strategy to promote the Li-ions transmission for single-crystalline LiNi 0.83 Co 0.11 Mn 0.06 O 2 (SCNCM) via Li 1.3 In 0.3 Ti 1.7 (PO 4 ) 3 (LITP) modification. It is noted that, as the fast Li-ion conductor, LITP can accelerate the Li-ions diffusion and alleviate the electrode–electrolyte side reaction simultaneously. More importantly, LITP can serve as the Li-ions regulator, ensuring the homogeneous distribution of Li-ions and minimizing the concentration difference at SCNCM surface. It can relieve the stress induced by the inconsistent Li-ions dispersion, which effectively decreases the degree of structural disordering and lattice mismatch at surface, eventually maintaining the high structure integrity during long-term cycling. As anticipated, even under the harsh testing conditions, the LITP modified SCNCM still can achieve a satisfied reversible capacity of 196.4 mAh g −1 under potential range of 2.75–4.6 V after 200 cycles at 25 °C in coin-type half-cells. Furthermore, it provides an extraordinary capacity retention of 88% in 2.75–4.3 V after 400 cycles at high temperature of 45 °C in pouch-type full-battery.

研究领域: 材料科学 · 电化学
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CHEMICAL ENGINEERING JOURNAL · 2018 · IF 6.735

Rapid and steady concentration gradient generation platform for an antimicrobial susceptibility test

Huanhuan Shi,Zhengli Hou,Yali Zhao,Kaixuan Nie,Bo Dong,Lemeng Chao,Shenghong Shang,Mengqiu Long,Zhengchun Liu

A simple microfluidic concentration gradient generator (MCG) was developed to create concentration gradients on a centimeter scale with a wide range of flow rates. Four groups of inlets (sample and buffer) were successively connected to the main channel to determine the location of inlets and the type of laminar flow and to create the concentration gradients. Nine micromixing channels were derived from the main channel to efficiently mix laminar flow. A micromixing channel whose mixing index was higher than that of a conventional serpentine mixing channel was designed by combining a square wave structure and microchannel sidewall grooves. A spindle-shaped chamber was set at the end of the mixing channel to observe the gradients. The computational fluid dynamic software Fluent was used to predict concentrations by calculating the average mass fraction at the cross section of each outlet. Theoretical simulations indicated that linear concentration gradients would be achieved within seconds in accordance with the fast micromixing principle at a flow rate of 2280 μL/min, and the gradient shape was steady regardless of the flow rate, which was affected by the location of inlet ports. The uniformity of the mass fraction achieved by the improved mixing channel was better than that of conventional serpentine micromixing channel. The theoretical simulations were verified through the generation of a concentration gradient of methylene blue water solution. Multiple concentrations of an antibacterial drug (ceftizoxime) generated by this MCG were utilized for an antimicrobial susceptibility test using Escherichia coli . Results revealed that the MCG showed potential for concentration gradient-related biochemical study.

研究领域: 生物工程 · 微生物学
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Advanced Energy Materials · 2022 ·Vol. 12 ·期 13 ·2103112 · IF 29.698

Li4Ti5O12 Coating on Copper Foil as Ion Redistributor Layer for Stable Lithium Metal Anode

Xiaosong Xiong,Wenqi Yan,Yusong Zhu,Lili Liu,Lijun Fu,Yuhui Chen,Nengfei Yu,Yuping Wu,Bin Wang,Rui Xiao

Lithium metal is regarded as the most promising electrode material for the next generation of energy storage devices. However, low coulombic efficiency and short cycle lifespan caused by the unstable electrode interface have hindered its practical application. Constructing artificial coatings on the anode is one of the most effective approaches for remedying this, but the practical effects are still limited due to their poor regulation of Li + ions transport and complex construction engineering. Herein, an “inverse concentration gradient” concept is put forward to improve the lithium metal anode, especially at high current density. A Li 4 Ti 5 O 12 artificial coating layer is fabricated on copper foil by a simple droplet coating method and a concentrated Li + ions region near the electrode interface in the coating layer is formed in situ after the initial activation process, which alleviates the effects of space charge regions generated by ion depletion on the growth of lithium dendrites. Coupled with high ionic conductivity and “zero strain” characteristics, stable dendrite-free cycling of lithium metal anodes is achieved even at 5 mA cm −2 in Li/Cu half cell. The unique concentration gradient design provides a new perspective for the interface regulation of advanced lithium metal anodes.

CAS / MDL: 13463-67-7
研究领域: 材料科学 · 电化学
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ACS Nano · 2024 · IF 15.8

All-Wood-Based Ionic Power Generator with Dual Functions for Alkaline Wastewater Reuse and Energy Harvesting

Kun Zhang,Xin Li,Chenyang Yan,Rongxiang Shi,Zhiqiang Fang,Songlin Zhou,Rong Cao,Junfei Tian

Water-induced electricity harvesting has gained much significance for energy sustainability. Bio-based hydrovoltaic materials increase the attractiveness of this strategy. Although promising, it faces a challenge due to its reliance on fresh water and its inherently low power output. Herein, the energy from alkalinity-gradient power generation demonstrated the feasibility of reuse of alkaline wastewater to develop an all-wood-based water-induced electric generator (WEG) based on ion concentration gradients. The intermittent water droplets bring about uneven distribution of electrolyte and endow delignified wood with the difference of ion concentration along aligned cellulose nanochannels, thus supplying electrical power. The practice of using alkali reservoirs, including industrial wastewater, further contributes to electricity generation. The cubic WEG with a side length of 2 cm can produce an ultrahigh open-circuit voltage of about 1.1 V and a short-circuit current of up to 320 μA. A power output of 6.75 μW cm–2 is correspondingly realized. Series-connected WEGs can be used as an energy source for commercial electronics and self-powered systems. Our design provides a double value proposition, allowing for sustainable energy generation and wastewater reuse.

研究领域: 材料科学 · 环境科学 · 能源技术
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SENSORS AND ACTUATORS B-CHEMICAL · 2019 · IF 6.393

High-throughput generation of a concentration gradient on open arrays by serial and parallel dilution for drug testing and screening

Xinlian Chen,Bing Ji,Xinghua Gao,Mengying Zhang,Chang Xue,Bingpu Zhou,Jinbo Wu

In this study, we successively and parallelly slide a solvent strip on a polydimethylsiloxane microwell array to dilute the solution within the microwells. A total of 60 concentration gradients were generated one by one along the sliding direction within minutes while simultaneously forming 60 microwells with the same concentration perpendicular to the sliding direction. Using theoretical calculations, simulated predictions and experimental verification, we could regulate the concentration gradient on the microwell array by tuning the parameters of the sliding head and sliding speed. Afterwards, we cultured human non-small cell lung cancer cells and produced an anticancer drug concentration gradient on the microwell array by this sliding method. The cell viability was examined to demonstrate the potential of this method for high-throughput cell-based drug testing and screening, and this open microwell array method may enable further analysis during a drug-screening process.

CAS / MDL: 518-47-8
研究领域: 生物工程 · 药理学 · 细胞生物学
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Journal of Materials Chemistry A · 2021 ·Vol. 9 ·期 46 ·26119-26126 · IF 12.732

Heat-triggered high-performance thermocells enable a self-powered forest fire alarm

Boyang Yu,Wei Yang,Jia Li,Wenke Xie,Hongrun Jin,Rong Liu,Hui Wang,Xinyan Zhuang,Bei Qi,Shiyou Liu,Liang Huang,Bin Hu,Jiangjiang Duan,Jun Zhou

Harvesting heat from fire itself to power wireless sensor networks has the potential to realize effective detection and alarm for forest fires. Thermocells based on the thermogalvanic effect offer an inexpensive and scalable way for heat-to-electricity conversion but challenged by their low performance. We demonstrate a boosted thermogalvanic effect by introducing concentration gradients into a thermocell, achieving a one order magnitude enhancement of output up to 45.9 W m−2. Using a heat-triggered membrane as the start switch, a thermocell which can hibernate in peacetime and awaken when fire occurs, is further obtained. A proof-of-concept device integrated from five units successfully detects precombustion and open fire to synchronously generate a high voltage of ∼2 V for driving an alarm. This system shows promise for combating the globally increasing forest fires.

研究领域: 能源材料学 · 环境科学
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