New paradigm of in situ characterization for next-generation CO2 electroreduction towards multi-carbon products over Cu-based catalysts

Customizing catalyst surface/interface structures for electrochemical CO2 reduction

“…For example, X-ray free-electron laser (XFEL) could be employed as the beam source to conduct XAS and IR measurements, which could afford useful information with higher quality within shorter test times than do synchrotron-radiation beam sources. 2 In addition, the combination of multiple in situ /operando techniques could also help to improve the accuracy and efficiency of characterization by simultaneously gathering information from the catalyst surface/interface, the reaction intermediates and the microenvironment. For example, the combination of operando infrared spectroscopy with time-of-flight mass spectrometry may offer more precise intermediate information for CO 2 RR.…”

“…Approximately half of the emission could be neutralized by land and ocean via the natural carbon cycle, and the other half accumulates in the Earth's atmosphere, resulting in pressing issues relating to environment and sustainability. 1–3 According to statistics from the Energy & Climate Intelligence Unit, more than 130 countries and regions have proclaimed the goal of “zero carbon” or “carbon neutrality”, and thus effective measures have to be taken to lower the atmospheric CO 2 concentration. 4,5 To this end, CO 2 conversion and utilization has been proposed as a potential solution to carbon neutrality.…”

“…21,22 In addition, only by looking deep into the surface/interface structures of catalysts can we establish the structure–performance relationship for CO 2 RR catalysis, which is of fundamental importance for developing more advanced electrocatalysts. 2,23…”

Atomically Precise Pd Species Accelerating CO2 Hydrodeoxygenation into CH4 with 100% Selectivity

“…In this context, CO 2 photoconversion into carbon-based fuels (CO, CH 4 , and so on) is a potential approach to mitigate the greenhouse effect and energy crisis . Among these carbon-based fuels, CO 2 photoreduction into CH 4 has attracted attention in academia and industry, since CH 4 with a calorific value of 890 kJ mol –1 can be utilized to directly fabricate chemical products and act as a living fuel. , However, the ultrahigh stability of CO 2 (the dissociation of CO = 750 kJ mol –1 ) results in a high energy barrier of CO 2 activation in thermodynamics, and hence CO 2 photoreduction into CH 4 encounters very poor activity. , Furthermore, the formation of CH 4 requires eight electrons, which is kinetically unfavorable compared to the generation of CO (two electrons), causing the generation of byproducts in the kinetics. − In this case, CO 2 photoreduction into CH 4 on traditional semiconductors suffers from low efficiency and unwanted byproducts due to the poor light absorption, slow charge separation efficiency, and surface reduction reaction. , Given this, many reports employ the broad-bandgap semiconductor to improve the efficiency of electron and hole separation for boosting the high-rate CO 2 reduction into CH 4 . Unfortunately, in the view of thermodynamics, the broad-bandgap semiconductor, such as ZnO, TiO 2 , and Ga 2 O 3 , usually can simultaneously match the reduction potential of various products, such as E CO2/CH4 = −0.24 V vs. NHE = 7 and E CO2/CO = −0.53 V vs. NHE = 7, resulting in uncontrollable selectivity. , In this case, construction of the cocatalyst (loading metal particle or metal oxides particles) helps to adjust the electronic structure of the semiconductor to narrow the distribution of products. − Nevertheless, as for these architectures, the presence of abundant microscopic structures causes it unable to determine the active species .…”

“…3,4 However, the ultrahigh stability of CO 2 (the dissociation of C�O = 750 kJ mol −1 ) results in a high energy barrier of CO 2 activation in thermodynamics, and hence CO 2 photoreduction into CH 4 encounters very poor activity. 5,6 Furthermore, the formation of CH 4 requires eight electrons, which is kinetically unfavorable compared to the generation of CO (two electrons), causing the generation of byproducts in the kinetics. 7−9 In this case, CO 2 photoreduction into CH 4 on traditional semiconductors suffers from low efficiency and unwanted byproducts due to the poor light absorption, slow charge separation efficiency, and surface reduction reaction.…”