Solar–Driven CO2 Conversion via Optimized Photothermal Catalysis in a Lotus Pod Structure

Wang, Hongmin; Fu, Shuting; Shang, Bo; Jeon, Sungho; Zhong, Yiren; Harmon, Nia J.; Choi, Chungseok; Stach, Eric A.; Wang, Hailiang

doi:10.1002/anie.202305251

Solar–Driven CO₂ Conversion via Optimized Photothermal Catalysis in a Lotus Pod Structure

Journal Article · Fri May 26 00:00:00 EDT 2023 · Angewandte Chemie (International Edition)

DOI:https://doi.org/10.1002/anie.202305251· OSTI ID:2421787

^[1]; Fu, Shuting ^[2]; Shang, Bo ^[2]; Jeon, Sungho ^[3]; Zhong, Yiren ^[2]; Harmon, Nia J. ^[2]; Choi, Chungseok ^[2]; Stach, Eric A. ^[3]; ^[2]

Yale University, New Haven, CT (United States); Yale University, West Haven, CT (United States); OSTI
Yale University, New Haven, CT (United States); Yale University, West Haven, CT (United States)
University of Pennsylvania, Philadelphia, PA (United States)

Photothermal CO₂ reduction is one of the most promising routes to efficiently utilize solar energy for fuel production at high rates. However, this reaction is currently limited by underdeveloped catalysts with low photothermal conversion efficiency, insufficient exposure of active sites, low active material loading, and high material cost. Herein, we report a potassium-modified carbon-supported cobalt (K⁺–Co–C) catalyst mimicking the structure of a lotus pod that addresses these challenges. As a result of the designed lotus-pod structure which features an efficient photothermal C substrate with hierarchical pores, an intimate Co/C interface with covalent bonding, and exposed Co catalytic sites with optimized CO binding strength, the K⁺–Co–C catalyst shows a record-high photothermal CO₂ hydrogenation rate of 758 mmol gcat^–1 h^–1 (2871 mmol gCo^–1 h^–1) with a 99.8 % selectivity for CO, three orders of magnitude higher than typical photochemical CO₂ reduction reactions. Here, we further demonstrate with this catalyst effective CO₂ conversion under natural sunlight one hour before sunset during the winter season, putting forward an important step towards practical solar fuel production.

View Accepted Manuscript (DOE)

Research Organization:: University of North Carolina, Chapel Hill, NC (United States)

Sponsoring Organization:: National Science Foundation (NSF); USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0021173

OSTI ID:: 2421787

Alternate ID(s):: OSTI ID: 1984911

Journal Information:: Angewandte Chemie (International Edition), Journal Name: Angewandte Chemie (International Edition) Journal Issue: 30 Vol. 62; ISSN 1433-7851

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

References (38)

Cobalt Plasmonic Superstructures Enable Almost 100% Broadband Photon Efficient CO ₂ Photocatalysis Feng, Kai; Wang, Shenghua; Zhang, Dake Advanced Materials, Vol. 32, Issue 24 https://doi.org/10.1002/adma.202000014	journal	May 2020
Solution–Liquid–Solid Growth and Catalytic Applications of Silica Nanorod Arrays Fang, Yaosi; Lv, Kangxiao; Li, Zhao Advanced Science, Vol. 7, Issue 13 https://doi.org/10.1002/advs.202000310	journal	May 2020
Atomic‐Level Reactive Sites for Semiconductor‐Based Photocatalytic CO ₂ Reduction Zhang, Yanzhao; Xia, Bingquan; Ran, Jingrun Advanced Energy Materials, Vol. 10, Issue 9 https://doi.org/10.1002/aenm.201903879	journal	January 2020
Photothermal Conversion of CO ₂ into CH ₄ with H ₂ over Group VIII Nanocatalysts: An Alternative Approach for Solar Fuel Production Meng, Xianguang; Wang, Tao; Liu, Lequan Angewandte Chemie International Edition, Vol. 53, Issue 43 https://doi.org/10.1002/anie.201404953	journal	July 2014
Tuning the CO ₂ Hydrogenation Selectivity of Rhodium Single‐Atom Catalysts on Zirconium Dioxide with Alkali Ions Li, Shang; Xu, Yuxing; Wang, Hengwei Angewandte Chemie International Edition, Vol. 62, Issue 8 https://doi.org/10.1002/anie.202218167	journal	January 2023
Cobalt‐Sputtered Anodic Aluminum Oxide Membrane for Efficient Photothermal CO ₂ Hydrogenation Lou, Deyue; Xu, Ao‐Bo; Fang, Yaosi ChemNanoMat, Vol. 7, Issue 9 https://doi.org/10.1002/cnma.202100162	journal	June 2021
All‐Earth‐Abundant Photothermal Silicon Platform for CO ₂ Catalysis with Nearly 100% Sunlight Harvesting Ability Zhang, Dake; Lv, Kangxiao; Li, Chaoran Solar RRL, Vol. 5, Issue 2 https://doi.org/10.1002/solr.202000387	journal	August 2020
Kinetics of reverse water gas shift (RWGS) reaction on metal disulfide catalysts Osaki, Toshihiko; Narita, Norichika; Horiuchi, Tatsuro Journal of Molecular Catalysis A: Chemical, Vol. 125, Issue 1 https://doi.org/10.1016/S1381-1169(97)00080-0	journal	October 1997
Promotion effects of potassium on the activity and selectivity of Pt/zeolite catalysts for reverse water gas shift reaction Yang, Xiaoli; Su, Xiong; Chen, Xiaodong Applied Catalysis B: Environmental, Vol. 216 https://doi.org/10.1016/j.apcatb.2017.05.067	journal	November 2017
Metal-organic framework-derived Ga-Cu/CeO2 catalyst for highly efficient photothermal catalytic CO2 reduction Deng, Bowen; Song, Hui; Peng, Kang Applied Catalysis B: Environmental, Vol. 298 https://doi.org/10.1016/j.apcatb.2021.120519	journal	December 2021
Photothermal functional material and structure for photothermal catalytic CO2 reduction: Recent advance, application and prospect Wang, Ziqi; Yang, Zhongqing; Kadirova, Zukhra C. Coordination Chemistry Reviews, Vol. 473 https://doi.org/10.1016/j.ccr.2022.214794	journal	December 2022
Product selectivity of photocatalytic CO2 reduction reactions Fu, Junwei; Jiang, Kexin; Qiu, Xiaoqing Materials Today, Vol. 32 https://doi.org/10.1016/j.mattod.2019.06.009	journal	January 2020
Highly active K-promoted Cu/β-Mo2C catalysts for reverse water gas shift reaction: Effect of potassium Xu, Jingjing; Gong, Xingxing; Hu, Rongrong Molecular Catalysis, Vol. 516 https://doi.org/10.1016/j.mcat.2021.111954	journal	November 2021
Concentrated solar energy applications using Fresnel lenses: A review Xie, W. T.; Dai, Y. J.; Wang, R. Z. Renewable and Sustainable Energy Reviews, Vol. 15, Issue 6 https://doi.org/10.1016/j.rser.2011.03.031	journal	August 2011
Understanding the Role of Inter- and Intramolecular Promoters in Electro- and Photochemical CO₂ Reduction Using Mn, Re, and Ru Catalysts Fujita, Etsuko; Grills, David C.; Manbeck, Gerald F. Accounts of Chemical Research, Vol. 55, Issue 5 https://doi.org/10.1021/acs.accounts.1c00616	journal	February 2022
High-Performance, Scalable, and Low-Cost Copper Hydroxyapatite for Photothermal CO2 Reduction Guo, Jiuli; Duchesne, Paul N.; Wang, Lu ACS Catalysis, Vol. 10, Issue 22 https://doi.org/10.1021/acscatal.0c03806	journal	November 2020
Microstructure Induced Thermodynamic and Kinetic Modulation to Enhance CO₂ Photothermal Reduction: A Case of Atomic-Scale Dispersed Co–N Species Anchored Co@C Hybrid Ning, Shangbo; Xu, Hua; Qi, Yuhang ACS Catalysis, Vol. 10, Issue 8 https://doi.org/10.1021/acscatal.9b04963	journal	February 2020
Deactivation and Stabilization Mechanism of Photothermal CO₂ Hydrogenation over Black TiO₂ Li, Yang; Zeng, Zhaojian; Zhang, Yuanming ACS Sustainable Chemistry & Engineering, Vol. 10, Issue 19 https://doi.org/10.1021/acssuschemeng.2c01081	journal	May 2022
Cu Atoms on Nanowire Pd/H _y WO _{3– x} Bronzes Enhance the Solar Reverse Water Gas Shift Reaction Li, Young Feng; Lu, Waylon; Chen, Kai Journal of the American Chemical Society, Vol. 141, Issue 38 https://doi.org/10.1021/jacs.9b08030	journal	September 2019
Plasmon-induced selective carbon dioxide conversion on earth-abundant aluminum-cuprous oxide antenna-reactor nanoparticles Robatjazi, Hossein; Zhao, Hangqi; Swearer, Dayne F. Nature Communications, Vol. 8, Issue 1 https://doi.org/10.1038/s41467-017-00055-z	journal	June 2017
Black indium oxide a photothermal CO2 hydrogenation catalyst Wang, Lu; Dong, Yuchan; Yan, Tingjiang Nature Communications, Vol. 11, Issue 1 https://doi.org/10.1038/s41467-020-16336-z	journal	May 2020
High-performance light-driven heterogeneous CO2 catalysis with near-unity selectivity on metal phosphides Xu, Yang-Fan; Duchesne, Paul N.; Wang, Lu Nature Communications, Vol. 11, Issue 1 https://doi.org/10.1038/s41467-020-18943-2	journal	October 2020
Grave-to-cradle upcycling of Ni from electroplating wastewater to photothermal CO2 catalysis Wang, Shenghua; Zhang, Dake; Wang, Wu Nature Communications, Vol. 13, Issue 1 https://doi.org/10.1038/s41467-022-33029-x	journal	September 2022
Engineered disorder in CO2 photocatalysis Li, Zhao; Mao, Chengliang; Pei, Qijun Nature Communications, Vol. 13, Issue 1 https://doi.org/10.1038/s41467-022-34798-1	journal	November 2022
Greenhouse-inspired supra-photothermal CO2 catalysis Cai, Mujin; Wu, Zhiyi; Li, Zhao Nature Energy, Vol. 6, Issue 8 https://doi.org/10.1038/s41560-021-00867-w	journal	July 2021
Highly stable, antiviral, antibacterial cotton textiles via molecular engineering Qian, Ji; Dong, Qi; Chun, Kayla Nature Nanotechnology, Vol. 18, Issue 2 https://doi.org/10.1038/s41565-022-01278-y	journal	December 2022
Cu2O nanocubes with mixed oxidation-state facets for (photo)catalytic hydrogenation of carbon dioxide Wan, Lili; Zhou, Qixing; Wang, Xin Nature Catalysis, Vol. 2, Issue 10 https://doi.org/10.1038/s41929-019-0338-z	journal	September 2019
Unified mechanistic understanding of CO2 reduction to CO on transition metal and single atom catalysts Vijay, Sudarshan; Ju, Wen; Brückner, Sven Nature Catalysis, Vol. 4, Issue 12 https://doi.org/10.1038/s41929-021-00705-y	journal	November 2021
Principles of photothermal gas-phase heterogeneous CO ₂ catalysis Ghoussoub, Mireille; Xia, Meikun; Duchesne, Paul N. Energy & Environmental Science, Vol. 12, Issue 4 https://doi.org/10.1039/C8EE02790K	journal	January 2019
Photothermal catalysts for hydrogenation reactions Liu, Huimin; Shi, Lizi; Zhang, Qijian Chemical Communications, Vol. 57, Issue 11 https://doi.org/10.1039/D0CC07144G	journal	January 2021
Shining light on CO ₂ : from materials discovery to photocatalyst, photoreactor and process engineering Dong, Yuchan; Duchesne, Paul; Mohan, Abhinav Chemical Society Reviews, Vol. 49, Issue 16 https://doi.org/10.1039/D0CS00597E	journal	January 2020
Construction of a Z-scheme heterojunction for high-efficiency visible-light-driven photocatalytic CO₂ reduction Zhang, Guoqiang; Wang, Zhiqi; Wu, Jinhu Nanoscale, Vol. 13, Issue 8 https://doi.org/10.1039/D0NR08442E	journal	January 2021
The reverse water gas shift reaction: a process systems engineering perspective González-Castaño, Miriam; Dorneanu, Bogdan; Arellano-García, Harvey Reaction Chemistry & Engineering, Vol. 6, Issue 6 https://doi.org/10.1039/D0RE00478B	journal	January 2021
Rationally designed nanoarray catalysts for boosted photothermal CO₂ hydrogenation Shen, Xukai; Li, Chaoran; Wu, Zhiyi Nanoscale, Vol. 14, Issue 32 https://doi.org/10.1039/D2NR02680E	journal	January 2022
High surface area siloxene for photothermal and electrochemical catalysis Su, Yize; Wang, Shenghua; Ji, Liang Nanoscale, Vol. 15, Issue 1 https://doi.org/10.1039/D2NR05140K	journal	January 2023
Net-zero emissions energy systems Davis, Steven J.; Lewis, Nathan S.; Shaner, Matthew Science, Vol. 360, Issue 6396 https://doi.org/10.1126/science.aas9793	journal	June 2018
Transition metal–free ketene formation from carbon monoxide through isolable ketenyl anions Jörges, Mike; Krischer, Felix; Gessner, Viktoria H. Science, Vol. 378, Issue 6626 https://doi.org/10.1126/science.ade4563	journal	December 2022
High-uniformity Memristor Arrays Based on Two-dimensional MoTe₂ for Neuromorphic Computing He, Huikai; Yang, Rui; Xia, Jian Journal of Inorganic Materials, Vol. 37, Issue 7 https://doi.org/10.15541/jim20210658	journal	January 2022

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