Correlating Oxidation State and Surface Ligand Motifs with the Selectivity of CO2 Photoreduction to C2 Products

Review Chemistry, Multidisciplinary

Solar fuels: research and development strategies to accelerate photocatalytic CO2 conversion into hydrocarbon fuels

Eunhee Gong et al.

Summary: This review highlights recent advances, challenges, and potential solutions in photocatalytic production of solar fuels from CO2, including discussions on various catalysts and reaction mechanisms.

ENERGY & ENVIRONMENTAL SCIENCE (2022)

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Article Chemistry, Physical

Tailoring the oxidation state of metallic TiO through Ti3+/Ti2+regulation for photocatalytic conversion of CO2 to C2H6

Baoxin Ni et al.

Summary: Adjusting the surface oxidation state distribution of metallic catalysts through co-doping can effectively promote the conversion of CO2 to C2 fuel.

APPLIED CATALYSIS B-ENVIRONMENTAL (2022)

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Article Chemistry, Physical

Dual Functionalized Interstitial N Atoms in Co3Mo3N Enabling CO2 Activation

Kai Feng et al.

Summary: The introduction of light elements into the interstitial sites of metals can enhance the catalytic performance by modifying the surface structure and electronic properties. In this study, N atoms were incorporated into the CoMo system to synthesize Co3Mo3N catalyst for reverse water-gas shift reaction. The enhanced catalytic performance of Co3Mo3N was attributed to the dual functions of interstitial N atoms, which provide additional sites for hydrogenation and weaken the binding ability of Mo to O-containing intermediates. The findings provide insights into the relationship between interstitial light element-promoted catalytic performance.

ACS CATALYSIS (2022)

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Review Physics, Condensed Matter

In-situ monitoring of dynamic behavior of catalyst materials and reaction intermediates in semiconductor catalytic processes

Zhen Fang et al.

Summary: This review highlights the importance of semiconductor photocatalysis in solar energy utilization and its implications for industrial, agricultural, and commercial development. The lack of understanding of catalyst evolution and reaction mechanism hinders the design of efficient and stable photocatalysts. Recent progress in in-situ exploration of catalyst materials and reaction intermediates is summarized, with a focus on microscopic imaging and spectroscopic characterization techniques. The challenges and problems in in-situ characterization are discussed, aiming to develop more advanced techniques to monitor accurate and realistic reaction processes and guide the design of advanced photocatalysts.

JOURNAL OF SEMICONDUCTORS (2022)

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Article Chemistry, Physical

Stabilizing intermediates and optimizing reaction processes with N doping in Cu2O for enhanced CO2 electroreduction

Chunliu Yan et al.

Summary: This study systematically reveals the mechanisms for enhanced CO2 electroreduction on nitrogen-doped Cu2O catalyst and demonstrates the importance of appropriate adsorption strength and modes of intermediates. The introduction of N into Cu2O significantly enhances CO2 adsorption capacity and binding strength of key intermediates, leading to increased production of CO and C2H4. The study also reveals that promoting the protonation step accelerates the formation of COOH center dot , facilitating the electroreduction of CO2.

APPLIED CATALYSIS B-ENVIRONMENTAL (2022)

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Article Chemistry, Multidisciplinary

Efficient Electrocatalytic Reduction of CO2 to Ethane over Nitrogen-Doped Fe2O3

Peng Chen et al.

Summary: This study reports a novel nitrogen-doped gamma-Fe2O3 electrocatalyst that can efficiently generate ethane in electrochemical reactions. The results showed that the enrichment of oxygen vacancies in the FeO1.5-nNn sites of the catalyst stabilized reaction intermediates and facilitated the generation of ethane by lowering the reaction energy barrier. This work provides a strategy for the design of efficient CO2 reduction catalysts.

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2022)

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Article Chemistry, Physical

Boosting Photocatalytic Nitrogen Fixation via Constructing Low-Oxidation-State Active Sites in the Nanoconfined Spinel Iron Cobalt Oxide

He Li et al.

Summary: In this study, a nanoconfined spinel iron cobalt oxide photocatalyst is developed to achieve both N2 enrichment and activation, leading to improved performance in the photocatalytic nitrogen reduction reaction.

ACS CATALYSIS (2022)

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Article Chemistry, Physical

Nitrogen doping of indium oxide for enhanced photocatalytic reduction of CO2 to methanol

Yuxiang Yang et al.

Summary: The nitrogen-doped indium oxide photocatalyst was found to be highly active and stable for the photocatalytic reduction of CO2 to methanol at ambient conditions. The nitrogen doping content can be tuned to improve the efficiency of methanol production. Nitrogen doping generates energy states and increases absorption and separation of photons. It also creates more active sites for CO2 adsorption and conversion. In addition, nitrogen doping enhances the activity of surface Lewis pairs, which further promotes CO2 adsorption and activation.

NANO ENERGY (2022)

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Review Chemistry, Multidisciplinary

Linking the Dynamic Chemical State of Catalysts with the Product Profile of Electrocatalytic CO2 Reduction

Jiali Wang et al.

Summary: Research has revealed the critical impact of dynamic chemical states on CO2RR selectivity, providing new insights for fundamental understanding and efficient electrocatalyst design.

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2021)

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Article Chemistry, Multidisciplinary

Asymmetric Triple-Atom Sites Confined in Ternary Oxide Enabling Selective CO2 Photothermal Reduction to Acetate

Juncheng Zhu et al.

Summary: This study introduces a novel design of materials with Metal-O-Metal triple-atom sites to facilitate CO2 reduction using photoinduced heat. Zn2GeO4 nanobelts, rich in oxygen vacancies, exhibit efficient acetate production and CO2 conversion under light illumination.

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2021)

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Article Chemistry, Multidisciplinary

Selective CO2 Photoreduction into C2 Product Enabled by Charge-Polarized Metal Pair Sites

Shan Zhu et al.

Summary: Selective CO2 photoreduction into a high-energy-density C-2 product is challenging, but can be enhanced by designing charge-polarized metal pairs sites. Theoretical calculations and experimental results confirm the asymmetric charge distribution on surface cobalt sites and the formation mechanism of the products. Electron-rich cobalt sites strengthen their interaction with oxygen in the intermediates, facilitating the formation of the desired product.

NANO LETTERS (2021)

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Article Multidisciplinary Sciences

Characterisation of oxygen defects and nitrogen impurities in TiO2 photocatalysts using variable-temperature X-ray powder diffraction

Christopher Foo et al.

Summary: TiO2-based powder materials have been extensively studied as efficient photocatalysts, especially nitrogen-doped TiO2, which exhibits visible-light absorption but the structure-activity relationship and photocatalytic mechanism remain unclear. A study on rutile, anatase and mixed phases revealed that nitrogen-doping improves photocatalytic activity and enhances oxygen vacancy formation. Additionally, a new cubic titanium oxynitride phase was identified in highly doped anatase, providing insight into the fundamental shift in absorption wavelength for excellent photocatalysis.

NATURE COMMUNICATIONS (2021)

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Review Chemistry, Multidisciplinary

Architectural Design for Enhanced C2 Product Selectivity in Electrochemical CO2 Reduction Using Cu-Based Catalysts: A Review

Changlong Xiao et al.

Summary: Electrochemical conversion of CO2 to value-added chemicals and fuels using Cu catalysts has shown promising potential, but poor product selectivity remains a major technical challenge for global applications. Tailoring the electrocatalyst architecture through nanotechnology principles can significantly impact the adsorption energetics of key intermediates and reaction pathways.

ACS NANO (2021)

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Article Chemistry, Physical

Coupling electrochemical CO2 conversion with CO2 capture

Ian Sullivan et al.

Summary: Electrochemical CO2 conversion into fuels or chemicals and CO2 capture from point or dilute sources are two important processes to address the gigaton challenges in reducing greenhouse gas emissions. Both processes are energy intensive, but synergistic coupling between them can improve energy efficiency and reduce costs, by eliminating the need for CO2 transport and storage or capture media regeneration.

NATURE CATALYSIS (2021)

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Article Multidisciplinary Sciences

Efficient photoelectrochemical CO2 conversion for selective acetic acid production

Xiaonong Wang et al.

Summary: This study achieves efficient conversion of CO2 to acetic acid by rational PEC device design, revealing the important role of Zn doping in Cu2O for selective catalytic CO2 conversion, and uncovering the equally crucial role of Au-loaded and N-doped TiO2 in initiating multi-electron CO2 reduction.

SCIENCE BULLETIN (2021)

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Article Chemistry, Multidisciplinary

Synergistic Effect of Cu Single Atoms and Au-Cu Alloy Nanoparticles on TiO2 for Efficient CO2 Photoreduction

Yangyang Yu et al.

Summary: The optimized photocatalyst developed in this study achieved record-high performance in synthesizing high-added-value solar fuels using sunlight. The synergistic function of Cu single atoms and Au-Cu alloy nanoparticles enhances the adsorption activation of CO2 and H2O, lowering the activation energy barrier for the formation of CH4 and C2H4. This concept of synergistic cocatalysts can be extended to other systems for the development of more effective catalysts.

ACS NANO (2021)

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Article Chemistry, Multidisciplinary

Understanding the Roles of Electrogenerated Co3+ and Co4+ in Selectivity-Tuned 5-Hydroxymethylfurfural Oxidation

Xiaohui Deng et al.

Summary: The study demonstrates that Co3+ and Co4+ species in Co-based electrocatalyst play distinct roles in the electrochemical oxidation of 5-hydroxymethylfurfural (HMF), with Co4+ being crucial for the initial oxidation of hydroxyl groups. By tuning the applied potential, selective production of 5-hydroxymethyl-2-furancarboxylic acid and 2,5-furandicarboxylic acid can be achieved. This work provides essential mechanistic insights for Co-catalyzed organic oxidation reactions and may guide the design of more efficient electrocatalysts.

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2021)

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Article Chemistry, Physical

Manipulating Cu Nanoparticle Surface Oxidation States Tunes Catalytic Selectivity toward CH4 or C2+ Products in CO2 Electroreduction

Qikui Fan et al.

Summary: A seed-assisted strategy for preparing Cu nanoparticles with PVP capping is presented in this study. The Cu NPs with sufficient PVP exhibit Cu-0 species, while those with deficient PVP form an oxide structure. Utilizing a flow cell configuration, Cu NPs deliver high Faradaic efficiencies for the CO2 reduction to CH4, outperforming many reported CO2 electrocatalysts. The presence of multicarbon products also demonstrates the crucial role of surface oxidation of Cu species in the CO2RR.

ADVANCED ENERGY MATERIALS (2021)

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Review Chemistry, Multidisciplinary

Regulating the oxidation state of nanomaterials for electrocatalytic CO2 reduction

Zhi-Zheng Wu et al.

Summary: Electrochemical carbon dioxide reduction reaction (CO2RR) converts CO2 into value-added chemicals and fuels, addressing renewable energy shortage and environmental pollution. Regulating the oxidation state of catalysts has been identified as an effective method for designing high-performing CO2RR catalysts that can influence catalyst activity and selectivity.

ENERGY & ENVIRONMENTAL SCIENCE (2021)

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Review Chemistry, Multidisciplinary

Photocatalytic and electrocatalytic transformations of C1 molecules involving C-C coupling

Shunji Xie et al.

Summary: This article provides a critical review on recent advances in photocatalytic and electrocatalytic conversions of major C1 molecules into C2+ compounds, and analyzes the structure-performance relationships and key factors to provide insights into the rational design of more efficient catalysts. The discussion includes the active species, reaction intermediates, and reaction or catalyst-functioning mechanism for a deeper understanding of the chemistry involved.

ENERGY & ENVIRONMENTAL SCIENCE (2021)

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Review Materials Science, Multidisciplinary