TiO<sub>2</sub>纳米粉在水中通过摩擦还原CO<sub>2</sub>

李鹏程; 唐重阳; 程亮; 胡永明; 肖湘衡; 陈万平

doi:10.7498/aps.70.20210210

摘要

纳米材料与特氟龙磁力搅拌棒之间的摩擦被发现可导致磁力搅拌条件下的染料降解. 本文对磁力搅拌条件下TiO₂纳米粉还原CO₂进行了研究. 在充有CO₂的100 mL石英反应器中, 在50 mL的水中分散1.00 g TiO₂纳米粉, 经过50 h磁力搅拌可产生6.65 × 10^–6 (体积分数, 下同) CO, 2.39 × 10^–6 CH₄和0.69 × 10^–6 H₂; 而如果没有TiO₂纳米粉, 则只能产生2.22 × 10^–6 CO和0.98 × 10^–6 CH₄. 对含有分散TiO₂纳米粉的水同时采用4个磁力搅拌棒, 50 h磁力搅拌产生的气体进一步提高到19.94 × 10^–6 CO, 2.33 × 10^–6 CH₄和2.06 × 10^–6 H₂. 基于TiO₂纳米粉通过摩擦吸收机械能并被激发产生电子-空穴对, 建立了TiO₂纳米粉对CO₂和水还原的催化机理. 本发现表明, 纳米材料能够通过摩擦利用机械能进行CO₂的还原, 从而为开发利用环境中的机械能提供了一个新的方向.

关键词:

摩擦 /
磁力搅拌 /
CO₂还原 /
TiO₂

Abstract

The friction between some nanomaterials and teflon magnetic stirring rods has recently been found responsible for dye degradation by magnetic stirring in dark. In this work, a study is conducted on the reduction of CO₂ by TiO₂ nanoparticles under magnetic stirring in water. In a 100-mL reactor filled with 50-mL water, 1.00-g TiO₂ nanoparticles and 1-atm CO₂, 50-h magnetic stirring results in the formation of 6.65 × 10^–6 (volume fraction) CO, 2.39 × 10^–6 CH₄ and 0.69 × 10^–6 H₂; while in a reactor without TiO₂ nanoparticles, the same magnetic stirring leads only 2.22 × 10^–6 CO and 0.98 × 10^–6 CH₄ to form. Four magnetic stirring rods are used simultaneously to further enhance the stirring, and 50-h magnetic stirring can form 19.94 × 10^–6 CO, 2.33 × 10^–6 CH₄, and 2.06 × 10^–6 H₂. A mechanism for the catalytic role of TiO₂ nanoparticles in the reduction of CO₂ and H₂O is established, which is based on the excitation of electron-hole pairs in TiO₂ by mechanical energy absorbed through friction. This finding clearly demonstrates that nanostructured semiconductors are able to utilize mechanical energy obtained through friction to reduce CO₂, thus providing a new direction for developing and utilizing the mechanical energy harvested from ambient environment.

Keywords:

作者及机构信息

1.
武汉大学物理科学与技术学院, 武汉　430072

2.
湖北大学物理与电子科学学院, 武汉　430062

通信作者: 陈万平, wpchen@whu.edu.cn

基金项目: 国家自然科学基金(批准号: U2067207)和国家重点研发计划(批准号: 2020YFB2008800)资助的课题

Authors and contacts

1.
School of Physics and Technology, Wuhan University, Wuhan 430072, China

2.
School of Physics and Electronic Science, Hubei University, Wuhan 430062, China

Corresponding author: Chen Wan-Ping, wpchen@whu.edu.cn

Funds: Project supported by the National Natural Science Foundation of China (Grant No. U2067207) and the National Key R&D Program of China (Grant No. 2020YFB2008800).

文章全文 : translate this paragraph

参考文献

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施引文献

图 1 二氧化钛纳米颗粒的SEM照片

Fig. 1. An SEM micrograph taken for as-received TiO₂ nanoparticles.

下载: 全尺寸图片幻灯片

图 2 单个磁力搅拌棒分别搅拌50 h溶解有CO₂的水及溶解有CO₂并分散有TiO₂纳米粉的水所产生的气体产物

Fig. 2. Gases produced from water dissolved with CO₂ through 50 h magnetic stirring using a PTFE (poly tetra fluoroethylene) magnetic stirring rod. There were no TiO₂ nanoparticles in water in the reference test.

下载: 全尺寸图片幻灯片

图 3 分别经过50, 100, 150 h磁力搅拌的气体产物, 在磁力搅拌中同时采用4个特氟龙磁力搅拌棒

Fig. 3. Gases produced from water dissolved with CO₂ through 50, 100 and 150 h, separately, magnetic stirring using four PTFE magnetic stirring rods.

下载: 全尺寸图片幻灯片

图 4 生成的气体体积分数与磁力搅拌时间的关系: 对溶解有CO₂并分散有TiO₂纳米粉的50 mL的水采用4个特氟龙磁力搅拌棒进行搅拌

Fig. 4. Stirring time dependence of CO, CH₄ and H₂ produced from water dissolved with CO₂ and dispersed with TiO₂ nanoparticles through magnetic stirring using four PTFE magnetic stirring rods.

下载: 全尺寸图片幻灯片

图 5 对含有TiO₂纳米粉的苯二甲酸钠溶液在室温及黑暗条件下用4个搅拌棒磁力搅拌后的荧光光谱(激发波长为315 nm)

Fig. 5. Fluorescence spectra (excitation wavelength: 315 nm) of sodium terephthalate solution containing TiO₂ nanoparticles after being magnetically stirred using four stirring rods at room temperature in dark.

下载: 全尺寸图片幻灯片

图 6 TiO₂纳米颗粒摩擦催化还原CO₂和水的示意图

Fig. 6. Schematic illustration of the tribocatalytic reduction of CO₂ and H₂O by TiO₂ nanoparticles under magnetic stirring.

下载: 全尺寸图片幻灯片

map

[1]	李冬冬, 王丽莉 2012 61 034212 Google Scholar Li D D, Wang L L 2012 Acta Phys. Sin. 61 034212 Google Scholar
[2]	李平, 李海金, 涂文广, 周勇, 邹志刚 2015 64 094209 Google Scholar Li P, Li H J, Tu W G, Zhou Y, Zou Z G 2015 Acta Phys. Sin. 64 094209 Google Scholar
[3]	吴化平, 令欢, 张征, 李研彪, 梁利华, 柴国钟 2017 66 167702 Google Scholar Wu H P, Ling H, Zhang Z, Li Y B, Liang L H, Chai G Z 2017 Acta Phys. Sin. 66 167702 Google Scholar
[4]	赵娟, 胡慧芳, 曾亚萍, 程彩萍 2013 62 158104 Google Scholar Zhao J, Hu H F, Zeng Y P, Cheng C P 2013 Acta Phys. Sin. 62 158104 Google Scholar
[5]	崔宗杨, 谢忠帅, 汪尧进, 袁国亮, 刘俊明 2020 69 127706 Google Scholar Cui Z Y, Xie Z S, Wang Y J, Yuan G L, Liu J M 2020 Acta Phys. Sin. 69 127706 Google Scholar
[6]	Ran J, Jaroniec M, Qiao S Z 2018 Adv. Mater. 30 1704649 Google Scholar
[7]	Kreft S, Wei D, Junge H, Beller M 2020 Energy Chem. 2 100044 Google Scholar
[8]	Wang X, Li Z, Yang X 2015 J. Mol. Sci. 31 190201
[9]	吴晔盛, 刘启, 曹杰, 李凯, 程广贵, 张忠强, 丁建宁, 蒋诗宇 2019 68 190201 Google Scholar Wu Y S, Liu Q, Cao J, Li K, Cheng G G, Zhang Z Q, Ding J N, Jiang S Y 2019 Acta Phys. Sin. 68 190201 Google Scholar
[10]	韩杰敏, 王梅, 仝召民, 马一飞 2019 无机材料学报 34 839 Google Scholar Han J M, Wang M, Tong Z M, Ma Y F 2019 J. Inorg. Mater. 34 839 Google Scholar
[11]	程广贵, 张伟, 方俊, 蒋诗宇, 丁建宁, Pesika N S, 张忠强, 郭立强, 王莹 2016 65 060201 Google Scholar Cheng G G, Zhang W, Fang J, Jiang S Y, Ding J N, Pesika N S, Zhang Z Q, Guo L Q, Wang Y 2016 Acta Phys. Sin. 65 060201 Google Scholar
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[13]	Deng J N, Kuang X, Liu R Y, Ding W B, Wang A C, Lai Y C, Dong K, Wen Z, Wang Y X, Wang L L, Qi H J, Zhang T, Wang Z L 2018 Adv. Mater. 30 1705918 Google Scholar
[14]	Wu J M, Chang W E, Chang Y T, Chang C K 2016 Adv. Mater. 28 3718 Google Scholar
[15]	Liang Z, Yan C F, Rtimi S, Bandara J 2019 Appl. Catal. B-Environ 241 256 Google Scholar
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[18]	Starr M B, Shi J, Wang X D 2012 Angew. Chem. Int. Ed. 51 5962 Google Scholar
[19]	You H, Wu Z, Zhang L, Ying Y, Liu Y, Fei L, Chen X, Jia Y, Wang Y, Wang F, Ju S, Qiao J, Lam C H, Huang H 2019 Angew. Chem. 58 11779 Google Scholar
[20]	Feng W, Yuan J, Zhang L, Hu W, Wu Z, Wang X, Huang X, Liu P, Zhang S 2020 Appl. Catal. B-Environ 277 119250 Google Scholar
[21]	Su R, Hsain H A, Wu M, Zhang D, Hu X, Wang Z, Wang X, Li F T, Chen X, Zhu L, Yang Y, Yang Y, Lou X, Pennycook S J 2019 Angew. Chem. 131 15220 Google Scholar
[22]	Yein W T, Wang Q, Liu Y, Li Y, Jian J H, Wu X H 2020 J. Environ. Chem. Eng. 8 103626 Google Scholar
[23]	Kang Z H, Qin N, Lin E Z, Wu J, Yuan B W, Bao D H 2020 J. Cleaner Prod. 261 121125 Google Scholar
[24]	Hao A, Ning X, Cao Y, Xie J, Jia D 2020 Mater. Chem. Front. 4 2096 Google Scholar
[25]	Wei Y, Zhang Y, Geng W, Su H, Long M 2019 Appl. Catal. B-Environ 259 118084 Google Scholar
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[34]	Zhao J, Chen L, Luo W, Li H, Wu Z, Xu Z, Zhang Y, Zhang H, Yuan G, Gao J, Jia Y 2020 Ceram. Int. 46 25293 Google Scholar
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[36]	Wu M, Lei H, Chen J, Dong X 2020 J. Colloid Interface Sci. 587 883
[37]	Ishibashi K I, Fujishima A, Watanabe T, Hashimoto K 2000 Electrochem. Commun. 2 207 Google Scholar
[38]	Baytekin B, Baytekin H T, Grzybowski B A 2012 J. Am. Chem. Soc. 134 7223 Google Scholar
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[40]	Kajdas C, Hiratsuka K 2009 Proc. Inst. Mech. Eng., Part J 223 827 Google Scholar
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[42]	Manini N, Mistura G, Paolicelli G, Tosatti E, Vanossi A 2017 Adv. Phys.: X 2 569
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[44]	Schneider J, Matsuoka M, Takeuchi M, Zhang J, Horiuchi Y, Anpo M, Bahnemann D W 2014 Chem. Rev. 114 9919 Google Scholar
[45]	Fujishima A, Zhang X, Tryk D 2008 Surf. Sci. Rep. 63 515 Google Scholar
[46]	Al-Mamoori A, Krishnamurthy A, Rownaghi A A, Rezaei F 2017 Energy Technol. 5 834 Google Scholar

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[16]	龚中良, 黄平. 界面摩擦过程非连续能量耗散机理研究. , 2008, 57(4): 2358-2362. doi: 10.7498/aps.57.2358
[17]	侯兴刚, 刘安东. V+注入锐钛矿TiO2第一性原理研究. , 2007, 56(8): 4896-4900. doi: 10.7498/aps.56.4896
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[20]	宋功保, 刘福生, 彭同江, 梁敬魁, 饶光辉. 金属离子掺杂对TiO2/白云母纳米复合材料中TiO2的颗粒形态及相组成的影响. , 2002, 51(12): 2793-2797. doi: 10.7498/aps.51.2793

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TiO₂纳米粉在水中通过摩擦还原CO₂