Construction of Z-type heterojunction BiVO4/Sm/α-Fe2O3 photoanode for selective degradation: Efficient removal of bisphenol A based on multifunctional Sm-doped modification

Electrocatalytic CO2 reduction is regarded as a green and promising technology because it can convert carbon dioxide into value-added fuel or chemicals in a flexible and sustainable way. This research aimed to comprehensively analyze the research hotspots and trends in the field of CO2 electroreduction from 2005 to 2022 using bibliometric methods based on the core database of Web of Science. The results showed that 4546 papers on CO2 electroreduction were retrieved from 2005 to 2022, with a clear increasing trend. The research direction was diversified, involving multiple disciplines, and it is a comprehensive research field. ACS Catalysis is the journal with the largest number of articles. China is the country with the largest number of documents and has made significant contributions to the development and progress of this field. Copper-based catalysts are still the research focus in recent years. It is of great practical significance to develop copper-based catalysts with high efficiency, low cost, high stability, and high selectivity for the preparation of C1 products.

https://www.mdpi.com/1996-1073/16/2/616/pdf?version=1673836522

A Scientometric Review of CO2 Electroreduction Research from 2005 to 2022

The development of efficient photoelectrodes to accelerate photoelectrochemical carbon dioxide reduction reaction (PEC-CO2RR) to obtain value-added chemicals or fuels is remarkably significant. Although Cu2O-based three-dimensional (3D) heterojunctions have emerged as promising materials for the selective generation of C2 products, they are still plagued by the stability of Cu+ in the Cu2O phase. In this work, we developed a binder-free Cu/Cu2O/CuO/Pd nanorods heterojunction via simple oxidation/reduction procedures to stabilize Cu+ in the Cu2O phase by incorporating high-work function Pd nanoparticles as a co-catalyst. The incorporated Pd not only stabilizes Cu+ through charge transfer from Cu2O to Pd but also enhances the stability of the *CO intermediate to improve C–C coupling for the formation of the C2 products, primarily acetate, and acetaldehyde. The Cu/Cu2O/CuO/Pd photoelectrode exhibits a superior Faradaic efficiency (FE) to produce acetate (21.4%) acetate and acetaldehyde (20.8%) at a negative potential of − 1.4 V (vs RHE), which are 3.5 and 19 times higher than that of Cu/Cu2O/CuO photoelectrode. Moreover, the Cu/Cu2O/CuO photoelectrode produces a maximum hydrogen gas evolution of ∼70% at − 1.2 V (vs RHE). Furthermore, compared to the Cu/Cu2O/CuO photoelectrode, the Cu/Cu2O/CuO/Pd photoelectrodes exhibit remarkable stability for a 5-h operation even at a higher negative applied potential of − 1.2 V vs RHE in CO2-saturated 0.1 M KHCO3. The stabilization of the Cu2O (111) phase is confirmed by the appearance of a characteristic X-ray diffraction and X-ray photoelectron peaks after PEC-CO2RR. These results indicate that the proposed high-stability Cu/Cu2O/CuO/Pd photoelectrode provides a new pathway to produce more C2 products of acetaldehyde and acetate. 

Binder-free Cu/Cu2O/CuO/Pd nanorods photoelectrode for regulating the faradaic efficiency for acetaldehyde and acetate production during photoelectrochemical CO2RR by stabilizing the Cu2O phase

Electrochemical CO2 reduction reaction (CO2RR) is an appealing strategy to alleviate the energy and environment issues caused by CO2 emission, and Cu-based electrodes show great potential in CO2 conversion. The wide product distribution makes Cu fail to be a high-efficiency catalyst for a specific product, and the competition with hydrogen evolution reaction is another critical issue. Various intermediates are involved in the CO2RR processes and some of them act as selective-dependent species, resulting in different products. Identifying the favorable pathways among those furcated from the key intermediates is crucial to target specific products. Herein, the key intermediates and competitive pathways furcated from them are discussed in detail. The *COOH and *OCHO can be formed upon CO2 activation, leading, respectively, to CO and HCOO− production. The *CO intermediate can competitively undergo hydrogenation and C-C coupling to, respectively, form *CHO/*COH and *OCCO. Aldehydes can lead to the formation of alcohols or hydrocarbons. The approaches to modulate the reaction tendency of these key intermediates are reviewed based on the characteristics of each possible pathway. The challenges and perspectives for the mechanism understanding are also discussed. 

Insights into selectivity modulation of electrochemical CO2 reduction reactions over Cu-based catalysts in terms of the key intermediates

The Cu-based photoelectrochemical CO2 reduction reaction (PEC–CO2RR) represents a convenient approach for producing value-added C2+ products, aiming to achieve carbon neutrality by reducing greenhouse gas emissions. However, these reactions typically suffer from limited selectivity. In this work, we fabricate Cu/Cu2O/CuO nanorod (CuR)-based heterojunction architectures integrated with Ag and Pd cocatalysts to boost the selectivity of C2+ products. The proposed Cu/Cu2O/CuO/Ag-Pd (CuR/Ag-Pd) photoelectrodes are used as photocathodes to generate a maximum Faradaic efficiency (FE) of C2+ products exceeding 53% by suppressing the hydrogen evolution reaction (HER). The FE improvement is approximately 22-fold (n-propanol), 12-fold (ethanol), 13-fold (acetaldehyde), and 6-fold (acetate) compared with CuR photoelectrodes operating at a negative applied potential of −1.8 V (vs. reversible hydrogen electrode, RHE). Conversely, the CuR photoelectrodes exhibit a maximum HER rate of ∼86% at −1.8 V (vs. RHE), higher than those of the CuR/Ag (54%) and CuR/Ag-Pd (35%) photoelectrodes. The superior PEC–CO2RR performance of CuR/Ag-Pd photoelectrodes is attributable to the higher electrochemical active surface area (6.7 mF/cm2) and faster charge transfer rate at the electrode/electrolyte interface owing to the presence of cocatalysts. In addition, the CuR/Ag-Pd photoelectrodes exhibit remarkable long-term stability retaining 70% of the initial performance even after a relatively more negative applied potential at −1.2 V. A comprehensive investigation into the changes in surface morphology, crystal structure, and elemental composition after PEC–CO2RR confirms the higher stability of CuR/Ag-Pd photoelectrodes. Thus, this work provides novel perceptions into the development of Cu-based heterojunction photoelectrodes integrated with Ag/Pd cocatalysts for improving the selectivity of C2+ products. 

Accelerating photoelectrochemical CO2RR selectively of C2+ products by integrating Ag/Pd cocatalysts on Cu/Cu2O/CuO heterojunction nanorods

Polyethyleneimine-reinforced Sn/Cu foam dendritic self-supporting catalytic cathode for CO2 reduction to HCOOH.

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Polyethyleneimine-reinforced Sn/Cu foam dendritic self-supporting catalytic cathode for CO2 reduction to HCOOH.