载流子浓度优化与动态掺杂提高n型PbS宽温域的热电性能  

Carrier concentration optimization and dynamic doping enhance the thermoelectric performance of n-type PbS over a wide temperature range

作　　者：侯正浩 崔秋娟 钱鑫 王淑芳[1] Zhenghao Hou;Qiujuan Cui;Xin Qian;Shufang Wang(College of Physics Science and Technology,Hebei Province Optoelectronic Information Materials Laboratory,Hebei University,Baoding 071002,China;College of Chemical Engineering,Shijiazhuang Key Laboratory of Low Carbon Energy Materials,Shijiazhuang University,Shijiazhuang 050035,China)

机构地区：[1]河北大学物理科学与技术学院,河北省光电信息材料重点实验室,保定071002 [2]石家庄学院化工学院,石家庄市低碳能源材料重点实验室,石家庄050035

出　　处：《科学通报》2025年第6期737-745,共9页Chinese Science Bulletin

基　　金：国家自然科学基金(52102234);河北省自然科学基金(E2024106001);河北省教育厅科学研究项目(QN2024263);石家庄学院博士科研启动基金(22BS006);河北省光电信息材料重点实验室补助经费(22567634H)资助。

摘　　要：硫化铅(PbS)基热电材料因其组成元素储量丰富、价格低廉、热稳定性高等优势而备受研究人员关注.目前关于PbS的研究主要聚焦于通过元素重掺杂提高其载流子浓度,以获得优良的中高温热电性能.然而,这种方法导致PbS近室温热电性能较差,严重制约了其在制冷领域的发展.本工作通过掺杂微量的GaBi,优化了n型PbS的载流子浓度,室温的功率因子达到21.70μW cm^(−1) K^(−2).同时,形成的Ga/Bi间隙原子与位错缺陷增强了声子散射,降低了PbS的晶格热导率,Pb_(0.99875)(GaBi)_(0.00125)S样品在300~773 K的平均ZT值达到0.58.为了进一步优化n型PbS在宽温域下的热电性能,通过引入Cu原子实现了载流子浓度的动态掺杂,Pb_(0.99875)(GaBi)_(0.00125)S+2%Cu样品的平均功率因子增加至17.6μW cm^(−1) K^(−2),平均ZT值进一步提升至0.65.本工作为优化PbS近室温区热电性能提供了新方法,对于推动PbS基热电材料在制冷领域的应用具有重要意义.Thermoelectric materials are essential for converting waste thermal energy directly into usable electrical energy and vice versa.This capability significantly enhances the efficiency of fossil energy conversion and contributes to environmental protection.Exceptional thermoelectric materials must exhibit both a high power factor and a low total thermal conductivity.Achieving a high power factor over a wide temperature range while maintaining a relatively low lattice thermal conductivity is critical for obtaining a high average figure of merit,which is vital for improving the efficiency of thermoelectric conversion across various temperatures.Optimizing a single thermoelectric parameter alone does not significantly improve the overall properties of the material.Therefore,contemporary thermoelectric research focuses on effectively regulating these parameters to enhance the ZT value.Lead chalcogenides,PbQ(where Q=Te,Se,or S),are mid-temperature thermoelectric materials renowned for their stable properties and excellent performance.PbTe,in particular,is a typical thermoelectric material that maintains a stable crystal structure and avoids phase transitions within its operational temperature range.It features a highly symmetric electronic band structure and a complex phonon band structure,which facilitates versatile control over its thermoelectric performance.However,the limited availability and high cost of tellurium in conventional PbTe compounds may constrain their widespread applications.As a result,PbS-based thermoelectric materials have attracted significant attention due to their abundant elemental resources,low cost,and high thermal stability.Current research on PbS focuses primarily on enhancing its carrier concentration through heavy element doping to achieve superior thermoelectric performance at medium to high temperatures.However,this approach often results in poor thermoelectric performance near room temperature,severely limiting its applications in thermoelectric cooling technologies.In this work,the car

关 键 词：热电材料 n型PbS 载流子浓度 动态掺杂 ZT值 

分 类 号：TB34[一般工业技术—材料科学与工程]