二维材料在光催化二氧化碳还原中的研究进展

doi:10.6023/A20080384

化学学报 ›› 2021, Vol. 79 ›› Issue (1): 10-22.DOI: 10.6023/A20080384 上一篇下一篇

综述

二维材料在光催化二氧化碳还原中的研究进展

陈钱¹, 匡勤^a^,^*(), 谢兆雄^a^,^*()

a 厦门大学化学化工学院厦门 361001

投稿日期:2020-08-21 发布日期:2020-09-24
通讯作者: 匡勤, 谢兆雄

作者简介:

陈钱, 分别于2016和2019年获得湖北大学学士学位和厦门大学硕士学位, 现为厦门大学博士生在读, 师从谢兆雄和匡勤, 主要研究兴趣为纳米光催化剂的设计合成、光催化分解水和光催化CO₂还原.

匡勤, 分别于2001和2008年于厦门大学获得学士和博士学位, 于2008年入职厦门大学化学系, 2009年获“中国化学会青年化学奖”, 2011年入选“教育部新世纪人才支持计划”以及首届“香江学者计划”, 当前主要研究方向为: (1)无机纳米晶表/界面可控合成及性能(光电、气敏、催化等)研究; (2)半导体-MOFs复合纳米材料的制备及应用; (3)纳米传感器的构筑及应用.

谢兆雄, 现担任厦门大学化学化工学院院长职务, 先后获得霍英东基金会优秀青年教师基金、教育部新世纪人才、国家杰出青年科学基金、卢嘉锡基金会优秀导师奖、“万人计划”科技创新领军人才、长江学者特聘等. 主要研究方向为: 表面与界面结构化学, 功能纳米材料结构化学, 功能晶体材料结构化学和新型传感器等方面. 在JACS,Angew. Chem. Int. Ed.,Nat. Commun.,Accounts Chem. Res.等国际著名期刊发表论文200余篇, 他引次数达到18185次, H-index为66, 入选科睿唯安全球高被引科学家.

* E-mail: qkuang@xmu.edu.cn; zxxie@xmu.edu.cn

基金资助:
国家重点研发计划(Nos. 2017YFA0206500); 国家重点研发计划(2017YFA0206801); 国家自然科学基金(Nos. 21671163); 国家自然科学基金(21773190); 国家自然科学基金(21721001); 国家自然科学基金(21931009)

Research Progress of Photocatalytic CO₂ Reduction Based on Two-dimensional Materials

Qian Chen¹, Qin Kuang^a^,^*(), Zhaoxiong Xie^a^,^*()

a College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361001, China

Received:2020-08-21 Published:2020-09-24
Contact: Qin Kuang, Zhaoxiong Xie
Supported by:
the National Key Research and Development Program of China(Nos. 2017YFA0206500); the National Key Research and Development Program of China(2017YFA0206801); the National Natural Science Foundation of China(Nos. 21671163); the National Natural Science Foundation of China(21773190); the National Natural Science Foundation of China(21721001); the National Natural Science Foundation of China(21931009)

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摘要/Abstract

近几十年来, 由温室效应所导致的气候变暖、海平面上升等环境问题日趋严重, 科学家们一直致力于研究可高效转化二氧化碳(CO₂)等温室气体的技术. 以太阳能为驱动力的光催化技术, 可将CO₂转化成甲烷、甲醇、甲酸或C₂₊等高附加值的碳氢燃料, 同时缓解温室效应和能源危机. 二维(2D)材料因具有超大的比表面积和独特的电子结构, 在光催化还原CO₂领域受到广泛的关注. 基于此, 作者综述了近年来2D材料实现CO₂分子高效转化的研究进展, 重点剖析了2D材料在光还原反应中的构-效关系, 并探讨了黑磷、石墨炔和共价有机框架化合物等新型2D材料作为CO₂光还原催化剂的发展潜力, 最后总体展望了CO₂光还原领域的研究前景和发展趋势.

关键词: 二维材料, 光催化, CO2光还原, 构-效关系

In past decades, global warming, sea level rising, and other climate problems caused by greenhouse effect are becoming more and more serious. Considerable efforts have been paid on developing new technology that can effectively reduce the atmospheric level of carbon dioxide (CO₂), the most representative one of greenhouse gases. Solar-driven conversion of CO₂ into high value-added hydrocarbon fuels is considered as the most promising approach to alleviate the current energy crisis and the rising CO₂ level. Benefiting from their high specific surface area and novel electronic structures, two dimensional (2D) materials have drawn intense interest in the field of CO₂ photoreduction. Herein, the latest development of 2D materials for photocatalytic CO₂ reduction is presented, with special emphasis given to the structure-activity relationship in catalytic reactions. The potentials of newly emerged 2D materials including black phosphorus, graphdiyne and covalent organic frameworks as the next generation photocatalysts for CO₂ reduction are then discussed. Finally, the opportunities and challenges in the field of CO₂ photoreduction are featured on the basis of its current development.

Key words: two-dimensional materials, photocatalysis, CO2 photoreduction, structure-activity relationship

引用此文

陈钱, 匡勤, 谢兆雄. 二维材料在光催化二氧化碳还原中的研究进展[J]. 化学学报, 2021, 79(1): 10-22.

Qian Chen, Qin Kuang, Zhaoxiong Xie. Research Progress of Photocatalytic CO₂ Reduction Based on Two-dimensional Materials[J]. Acta Chimica Sinica, 2021, 79(1): 10-22.

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图/表 14

Reactions	E ⁰redox/V (vs. NHE)
CO₂+e^–→CO₂ ^•–	–1.85
CO₂+2H⁺+2e^–→HCOOH	–0.61
CO₂+2H⁺+2e^–→CO+H₂O	–0.53
CO₂+4H⁺+4e^–→HCHO+H₂O	–0.48
CO₂+4H⁺+4e^–→C+2H₂O	–0.20
CO₂+6H⁺+6e^–→CH₃OH+H₂O	–0.38
CO₂+8H⁺+8e^–→CH₄+2H₂O	–0.24
2CO₂+12H⁺+12e^–→C₂H₄+4H₂O	–0.34
2CO₂+12H⁺+12e^–→C₂H₅OH+3H₂O	–0.33
2CO₂+14H⁺+14e^–→C₂H₆+4H₂O	–0.27
2H⁺+2e^–→H₂	–0.42

表1. CO2光还原反应的主要产物及对应的还原电极电势(相对于标准氢电极), pH=7水溶液, 25 ℃[ 20]

Table 1. The main products of CO2 reduction and corresponding reduction potentials with reference to NHE at pH 7 in aqueous solution, 25 ℃[ 20]

图1. 二维材料家族[ 21]

Figure 1. 2D material family[ 21]

图2. 二维材料作为CO2光还原催化剂的优势所在[48]

Figure 2. The advantages of 2D materials as photocatalysts for CO2 reduction[48]

图3. 光催化CO2还原的反应步骤示意图[8]

Figure 3. Schematic illustration of reaction steps in photocatalytic CO2 reduction[8]

图4. 超薄TiO2的 (a)扫描电镜图. (b)超薄TiO2与块状TiO2的电荷分布示意图. (c)超薄TiO2和(d)块状TiO2的态密度计算. (e)超薄TiO2和(f)块状TiO2上甲酸产量随反应时间的变化关系图[51].

Figure 4. (a) SEM of ultrathin TiO2. (b) The charge distribution of ultrathin and bulk TiO2, the calculated density of states of (c) ultrathin TiO2 and (d) bulk TiO2. Time dependent HCOOH yields on (e) ultrathin TiO2and (f) bulk TiO2 [51].

图5. 金属氧化物和硫化物相对于真空能级和标准氢电极的禁带宽度和带边位置[77]

Figure 5. Band gaps and band-edge positions with respect to the vacuum level and NHE for metal oxides and chalcogenides[77]

图6. 单层BiOBr的 (a)透射电镜图和(b)结构模型图. (c)块状和单层BiOBr的能带结构示意图. 块状和单层BiOBr上(d) CO和(e) CH4的生成速率[62]. (f)含氧空位的BiOBr的紫外-可见漫反射光谱图. (g)含氧空位、不含氧空位以及块状BiOBr催化剂上CO的生成速率[63].

Figure 6. (a) TEM image and (b) structural mode of monolayer BiOBr. (c) Schematic illustration of band gap energy structures of bulk and monolayer BiOBr. The evolution rates of (d) CO and (e) CH4 on bulk and monolayer BiOBr, respectively[62]. (f) UV-vis diffuse reflectance spectroscopy of BiOBr with VO. (g) CO evolution rate on BiOBr with VO, without VO and bulk BiOBr, respectively[63].

图7. 2D/2D Ni3HITP2 MOF/rGO二维异质结: (a)低分辨率透射电镜图, (b)高分辨率透射电镜图, (c)能带结构和电荷转移示意图. 光催化CO2还原活性图: (d)单位时间内CO和H2的产量, (e)单位质量样品的CO产量[65].

Figure 7. 2D/2D Ni3HITP2 MOF/rGO heterostructures: (a) low and (b) high resolution TEM image, (c) schematic illustration of band gap structures and charge migration. Photocatalytic CO2 reduction performance: (d) CO and H2 yields on per hour of time, (e) CO yield on per gram of catalysts, respectively[65].

图8. (a) LDHs的结构示意图[84]. ZnAl-LDH体系表征图: (b), (c)和(d)分别为三种不同尺寸和厚度的ZnAl-LDH的透射电镜图. (e) CO2的吸附能. (f)三种不同尺寸和厚度样品的CO产量对比图[33].

Figure 8. (a) Structure illustration of LDHs[84]. Characterization results of ZnAl-LDH: (b), (c) and (d) TEM images of three ZnAl-LDH samples with different size and thickness, respectively. (e) Adsorption energy of CO2. (f) CO yields on above mentioned three samples with different size and thickness[33].

图9. 从原始的211, 312和413相MAX转变成MXene的结构演变示意图[85].

Figure 9. Schematic illustration of structure evolution of MXene from the pristine MAX 211, 312 and 413 phases[85].

图10. 石墨烯基光催化剂用于CO2光还原[87].

Figure 10. Graphene-based photocatalysts for CO2 photoreduction[87].

图11. (a)富氮前驱体高温聚合生成石墨相氮化碳的流程示意图[89]. (b)含/不含碳空位的g-C3N4上CO2活化的吉布斯自由能. (c)含有不同浓度碳空位的g-C3N4的光催化活性与选择性[28]. (d), (e), (f) 内嵌Ti-O物种的g-C3N4纳米片的透射电镜图; (g) g-C3N4、TiO2以及内嵌Ti-O物种的g-C3N4纳米片的活性对比图[29].

Figure 11. (a) Synthesis of g-C3N4 by thermal polymerization of N-rich molecular precursors[89]. (b) Gibbs free energy diagrams for the activation of CO2 on g-C3N4 with/without VC. (c) Photocatalytic activity and selectivity of g-C3N4with different concentrations of VC [28]. (d), (e) and (f) TEM images of g-C3N4 NSs implanted with Ti-O species; (g) the time dependent CO productions on the pristine g-C3N4, TiO2 and g-C3N4 NSs implanted with Ti-O species[29].

图12. (a)h-BN模型图[21]. 碳掺杂h-BN的相关表征: (b) BCN-30的透射电镜图, (c)h-BN和BCN-30的电子结构, (d) BCN-30的CO2光还原活性和选择性[26]. 氧掺杂BN的相关表征: (e) O-BN的透射电镜图, (f) O-BN和h-BN的CO2光还原活性对比图, (g) CO2在O-BN和h-BN上的吸附能[27].

Figure 12. (a) Structure mode of h-BN[21]. Characterization results of C-doped h-BN: (b) TEM image of BCN-30, (c) electron structures of h-BN and BCN-30, (d) CO2 photoreduction activity and selectivity of BCN-30[26]. Characterization results of O-doped h-BN: (e) TEM image of O-BN, (f) CO2 photoreduction activity of O-BN and the pristine h-BN, (g) adsorption energies of CO2 on O-BN and the pristine h-BN[27].

图13. 二维异质结的结构示意图: (a)范德华异质结, (b)平面异质结[ 115] . Ti3C2-Bi2WO6范德华异质结的相关表征: (c), (d)透射电镜图, (e)含不同Ti3C2载量的复合材料的光催化CO2还原活性[ 118] . SnS2-SnO2平面异质结的相关表征: (f)透射电镜图及元素排布示意图, (g)含不同SnO2组分的样品的CO2还原活性[ 25] .

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二维材料在光催化二氧化碳还原中的研究进展

Research Progress of Photocatalytic CO₂ Reduction Based on Two-dimensional Materials

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二维材料在光催化二氧化碳还原中的研究进展

Research Progress of Photocatalytic CO2 Reduction Based on Two-dimensional Materials

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Research Progress of Photocatalytic CO₂ Reduction Based on Two-dimensional Materials