Recently, bismuth sulfide (Bi2S3) has attracted much attention in the thermoelectric community owing to its abundance, low cost, and advanced properties. However, its poor electrical transport properties have prevente...Recently, bismuth sulfide (Bi2S3) has attracted much attention in the thermoelectric community owing to its abundance, low cost, and advanced properties. However, its poor electrical transport properties have prevented Bi2S3 devices from realizing high thermoelectric performance. In this work, our motivation is to decrease the large electrical resistivity, which is recognized as the origin of the low ZT value in undoped Bi2S3. We combined melting and spark plasma sintering (SPS) in a continuous fabrication process to produce Bi2S3–xSex (x = 0, 0.09, 0.15, 0.21) and Bi2S2.85–ySe0.15Cly (y = 0.0015, 0.0045, 0.0075, 0.015, 0.03) samples. Our results show that Se alloying at S sites can narrow the band gap and activate intrinsic electron conduction, leading to a high power factor of ~2.0 μW·cm–1·K–2 at room temperature in Bi2S2.85S0.15, about 100 times higher than that of undoped Bi2S3. Moreover, our further introduction of Cl atoms into the S sites resulted in a second-stage optimization of carrier concentration and simultaneously reduced the lattice thermal conductivity, which contributed to a high ZT value of ~0.6 at 723 K for Bi2S2.835Se0.15Cl0.015. Our results indicate that high thermoelectric performance could be realized in Bi2S3 with earth-abundant and low-cost elements.展开更多
基金supported by the National Key Research and Development Program of China under Grant No. 2018YFB0703600, the National Natural Science Foundation of China under Grant Nos. 51772012, 51671015, and 51571007the Beijing Municipal Science & Technology Commission under Grant No. Z171100002017002+2 种基金the Shenzhen Peacock Plan team under Grant No. KQTD2016022619565991111 Project under Grant No. B17002supported by the High Performance Computing Center of Henan Normal University.
文摘Recently, bismuth sulfide (Bi2S3) has attracted much attention in the thermoelectric community owing to its abundance, low cost, and advanced properties. However, its poor electrical transport properties have prevented Bi2S3 devices from realizing high thermoelectric performance. In this work, our motivation is to decrease the large electrical resistivity, which is recognized as the origin of the low ZT value in undoped Bi2S3. We combined melting and spark plasma sintering (SPS) in a continuous fabrication process to produce Bi2S3–xSex (x = 0, 0.09, 0.15, 0.21) and Bi2S2.85–ySe0.15Cly (y = 0.0015, 0.0045, 0.0075, 0.015, 0.03) samples. Our results show that Se alloying at S sites can narrow the band gap and activate intrinsic electron conduction, leading to a high power factor of ~2.0 μW·cm–1·K–2 at room temperature in Bi2S2.85S0.15, about 100 times higher than that of undoped Bi2S3. Moreover, our further introduction of Cl atoms into the S sites resulted in a second-stage optimization of carrier concentration and simultaneously reduced the lattice thermal conductivity, which contributed to a high ZT value of ~0.6 at 723 K for Bi2S2.835Se0.15Cl0.015. Our results indicate that high thermoelectric performance could be realized in Bi2S3 with earth-abundant and low-cost elements.