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

doi:10.6023/A20080384

Acta Chimica Sinica ›› 2021, Vol. 79 ›› Issue (1): 10-22.DOI: 10.6023/A20080384 Previous Articles Next Articles

Review

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)

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

Cite this article

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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Fig. & Tab. 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

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

Figure 1. 2D material family[ 21]

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

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

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].

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

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].

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].

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].

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

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

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].

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].

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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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