微纳粉体样品库高通量并行合成的研究进展

doi:10.15541/jim20210247

摘要/Abstract

摘要：

高通量制备可通过并行合成策略快速获得大量成分准连续或梯度变化的样品, 从中筛选出具有最佳成分与性能的目标材料, 将传统的“试错法”研发模式变革为系统寻优的新模式, 可以显著提高研发效率。高通量制备实验还可与材料计算和机器学习等虚拟实验相辅相成, 验证计算结果, 并为数据挖掘和应用提供更丰富的实验基础。本文综述了微纳粉体样品库高通量并行合成方法和进展, 这些典型的高通量制备方法为功能粉体材料研发工作者加速实验进程提供了新思路和高效合成路径, 已应用于催化剂、荧光粉、红外辐射材料、电催化材料等的快速发现和优选, 并将不断扩大应用领域和规模, 凸显其先进性和应用价值。

关键词: 并行合成, 高通量, 微纳粉体, 阵列样品库, 前驱物输运, 综述

Abstract:

The high-throughput preparation of material library can quickly obtain a large number of samples with quasi-continuous or gradient change of composition by parallel synthesis strategy, and screen the target materials with the best composition and performance. The traditional “trial and error” mode has been transformed into a new mode of system optimization in materials exploration. At the same time, high-throughput preparation experiments can complement virtual experiments such as material computing and machine learning to verify the calculation results, and provide an abundant experimental database for data mining and application. This paper reviews the parallel synthesis methods of micro-nano powder and their progress, which provide new ideas and efficient synthesis routes for the functional materials scientists to accelerate the experimental process. The mentioned high-throughput experimental methods have been applied to the rapid discovery, optimization and performance improvement of new materials, such as catalysts, phosphors, infrared irradiative materials, and so on, which is expected to expand the application area and scale, highlighting its advancement and value.

Key words: parallel synthesis, high throughput, micro-nano powder, sample library, precursor transport, review

中图分类号:

TQ050

刘茜, 王家成, 周真真, 徐小科. 微纳粉体样品库高通量并行合成的研究进展[J]. 无机材料学报, 2021, 36(12): 1237-1246.

LIU Qian, WANG Jiacheng, ZHOU Zhenzhen, XU Xiaoke. Research Progress on High Throughput Parallel Synthesis of Micro-nano Powders Libraries[J]. Journal of Inorganic Materials, 2021, 36(12): 1237-1246.

图/表 12

图1 光催化剂样品库可见光辐照催化活性快速评价装置[9]

Fig. 1 Front view of the experimental setup for visible-light irradiation of the photocatalysts libraries[9] Ⓐ Array of lamps (Osram Dulus S G23, 11W); Ⓑ Bath of frosted glass filled with 1 mol/L K2CrO4 solution; Ⓒ Library of 45 HPLC flasks arranged in five columns and nine rows; Ⓓ Orbital shaker (Heidolph Titramax 100)

图2 (a)组合溶液喷射系统示意图(主要包括微压电喷头, 原液储存容器, x-y移动台, 阵列微反应器等)[12]; (b)溶胶-凝胶合成装置主体示意图(1-箱体, 内置梯度温控; 4-摇动电机; 5-支撑杆; 7-反应腔; 8-微反应器阵列)[16]

Fig. 2 (a) Schematic diagram of drop-on-demand inkjet delivery system (mainly with micro-piezoelectric inkjet head, solution reservoir, x-y moving stage, microreactor and substrate)[12]; (b) schematic diagram of Sol-Gel device (1-box with temperature controlling insides; 4-shaking motor; 5-support rod; 7-reaction chamber; 8-microreactor array)[16]

图3 (a)代表性的三激光束并行加热系统示意图(主要包括激光源、反射镜、阵列样品支撑和移动台、计算机和控制器等)[21], (b)三通道光谱仪示意图(主要包括光纤光谱模块、光谱校准模块、LE和LED光源、阵列样品支撑和移动台等)[22]

Fig. 3 (a) Schematic diagram of a typical triple-laser-beam parallel heating system(mainly including laser sources, reflectors, sample library holder and moving platform, computer and controllers)[21]; (b) Schematic diagram of a representative triple channel optical spectrometer(mainly including fiber optical spectrometer, spectral calibration device, modular LE and LED excitation source, sample library holder and moving platform)[22]

图4 由聚四氟乙烯制成的单层100通道水热合成粉体装置图(可沿纵向堆叠)[23]

Fig. 4 View of the multi-autoclave showing the mode of stacking of the Teflon blocks and one of the alternative designs using Teflon inserts which can be stacked vertically[23]

图5 (a)高通量连续水热流合成纳米晶系统示意图; (b)冰冻干燥并经1000 ℃煅烧处理的系列样品分别填入聚四氟乙烯三角形样品盒用于后续表征示意图[29]

Fig. 5 (a) Schematic layout of the high-throughput hydrothermal (HiTCH) flow synthesis system, and (b) shematic of freeze-dried powders fired at 1000 ℃ and filled into a PTFE triangular holder[29]

图6 (a)陶瓷基片-铜网-金属掩膜三层结构微型反应装置示意图; (b)实物照片; (c)合成粉体转入一个与陶瓷微反应器基板具有相同几何尺寸的塑料基板, 塑料基板凹坑深度2 mm; (d)用金属压头将粉体压实[39]

Fig. 6 Schematic diagram (a) and photograph (b) of the ceramic substrate-copper net-metal mask microreactor array, (c) a plastic substrate with the same predrilled shallow wells (2 mm in depth) as the library, then flipped over the synthesized powders into the shallow wells, and (d) a metal plate used to compact powders[39]

图7 制备三种成分任意组合反应的微流控芯片示意图[42]

Fig. 7 Schematic diagram of microfluidic chip for synthesis of three-elements compounds[42]

图8 基于微流控芯片的光催化剂筛选系统设计图(a), 具有楔形机构的多通道微流控芯片示意图(b), 催化剂装载示意图(c)和催化剂筛选过程示意(d)[43]

Fig. 8 Setup of the microchip-based photocatalyst screening system (a), schematic diagram of the multi-channel array ship with a wedge structure in each channel (b), schematic diagram of the catalyst loading (c), and illustration of the catalyst screening procedure (d)[43] (d1) Loading catalyst particles in the microchannel to form the column; (d2) Introducing MB solution into the channel and recording the initial channel image; (d3) MB degradation under UV light; (d4) Recording the channel image after definite time

图9 基于微流控芯片的溶液成分及温度控制平台(包括2个入液口和20个出液口(a), 微反应器阵列细节(包括100个孔位和5个温度梯度)以及圣诞树型的微流控芯片结构(b)[48]

Fig. 9 Photos of the microfluidic-based composition and temperature controlling platform with two inlets and 20 outlets (a), details of the micro-reactor arrays (120-230 ℃, 100 holes) and microfluidic chip having Christmas-tree-type structure (b)[48]

图10 (Sr,Ca,Ba,Mg)2Si5N8:Eu2+组合样品库的发光强度和色坐标筛选结果: (a) (Ca,Sr,Mg)2Si5N8:Eu2+体系; (b) (Ca,Sr,Mg)2Si5N8:Eu2+体系; (c) (Ca,Sr,Ba)2Si5N8:Eu2+体系; (d) (Sr,Ba,Mg)2Si5N8:Eu2+体系[49]

Fig. 10 Ternary combi-chem libraries for (a) (Ca,Sr,Mg)2Si5N8: Eu2+, (b) (Ca,Sr,Mg)2Si5N8:Eu2+, (c) (Ca,Sr,Ba)2Si5N8:Eu2+, and (d) (Sr,Ba,Mg)2Si5N8:Eu2+ in terms of photoluminescent intensity and color chromaticity[49] Actual photos taken under 365 nm excitations are also presented

图11 高通量配料装置内部结构(a),固态粉体配料(b)及操作(c)流程示意图[53]

Fig. 11 Internal structure(a), schematic diagram (b) and operation flow chart (c) of the high throughput equipment[53]

图12 高通量电场辅助燃烧合成系统示意图[55]

Fig. 12 Schematic diagram of high-throughput electric field-assisted combustion synthesis system[55] 4×4 array sintered samples

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