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Science Bulletin 64 (2019) 1805–1816

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Science Bulletin 64 (2019) 1805–1816 Science Bulletin 64 (2019) 1805–1816 Contents lists available at ScienceDirect Science Bulletin journal homepage: www.elsevier.com/locate/scib Review Pushing the activity of CO2 electroreduction by system engineering ⇑ Hao Shen, Zhengxiang Gu, Gengfeng Zheng Laboratory of Advanced Materials, Department of Chemistry and Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Fudan University, Shanghai 200438, China article info abstract Article history: As a promising technology that may solve global environmental challenges and enable intermittent Received 10 July 2019 renewable energy storage as well as zero-carbon-emission energy cycling, the carbon dioxide reduction Received in revised form 15 August 2019 reaction has been extensively studied in the past several years. Beyond the fruitful progresses and inno- Accepted 22 August 2019 vations in catalysts, the system engineering-based research on the full carbon dioxide reduction reaction Available online 26 August 2019 is urgently needed toward the industrial application. In this review, we summarize and discuss recent works on the innovations in the reactor architectures and optimizations based on system engineering Keywords: in carbon dioxide reduction reaction. Some challenges and future trends in this field are further dis- CO reduction 2 cussed, especially on the system engineering factors. Electrocatalysis Ó Flow-cell electrolyzer 2019 Science China Press. Published by Elsevier B.V. and Science China Press. All rights reserved. Catalytic reactor engineering Artificial photosynthesis 1. Introduction cycling, the photochemical or electrochemical catalytic reduction of CO2 started to be demonstrated in 1970s and has achieved The excessive dependence of fossil energy in daily life and the extensive attention in the past decade [6–8]. Researchers have resulting environmental pollution of massive emissions of carbon learnt from and then mimicked the natural photosynthesis process dioxide (CO2), one of the major greenhouse gases, is a series of glo- of green plants, and proposed a new process that allows clean bal challenges that are facing the human society today [1]. On the energy to drive electrocatalytic CO2 reduction to generate different one hand, with the rapid economic development and population molecules with energy storage [9]. This process is also known as growth, the global energy demand is continuously increasing. the artificial photosynthesis (AP) process. Different artificial photo- Fossil fuels are limited as non-renewable resources, resulting in synthesis systems with diverse electrochemical reactions have an increased energy crisis [2]. On the other hand, due to the large been developed and studied to convert CO2 into value-added consumption of fossil fuels, the emitted CO2 is accumulating in the chemicals or fuels, including photocatalytic [10,11], photoelectro- atmosphere year by year, and the continuous increase of artificial chemical [12–14], electrocatalytic [15–17], and biocatalytic reac- CO2 emissions has caused serious environmental problems [3,4]. tions [18]. On May 11th, 2019, a historic high CO2 level of 415.26 ppm was Among various artificial photosynthesis systems, the develop- recorded by Mauna Loa Observatory in Hawaii, which sounded ment of solar-driven electrocatalytic CO2 reduction reaction the alarm for mankind once again (https://www.research.noaa. (CO2RR) is widely considered to have the potential for large-scale gov/News/Scientist-Profile/ArtMID/536/ArticleID/2461/Carbon- practical applications with high efficiency and low cost [19,20], dioxide-levels-hit-record-peak-in-May). If no active and effective and has thus become a research hotspot of various artificial photo- actions were to be taken, the current human development path synthesis devices. These successful researches on solar cells have would become greatly affected in the near future. Thus, technolo- efficiently pushed the solar-to-electric energy conversion to a high gies that use renewable energies on a large scale to replace the level of 39.2% for multi-junction cell and 29.1% for single-junction existing fossil energy-based energy structures are urgently needed. cell [21]. This artificial photosynthetic system is mainly subject to Among them, the efficient renewable energy conversion and stor- the low activity and selectivity of electrocatalytic CO2 reduction age methods should exist in the core position [5]. reactions [22]. Furthermore, the realization of high activity and As a promising technology that may enable the intermittent high selectivity of CO2RR requires comprehensive innovation and renewable energy storage and zero-carbon-emission energy optimization from electrocatalysts to catalytic systems. Substantial research developments on electrocatalyst innova- tion have been made in order to solve the problem of poor activity SPECIAL ISSUE: Emerging Investigators 2019 ⇑ Corresponding author. and selectivity of electrocatalytic CO2RR [23–25]. Both homoge- E-mail address: [email protected] (G. Zheng). neous and heterogeneous catalysts have been extensively studied https://doi.org/10.1016/j.scib.2019.08.027 2095-9273/Ó 2019 Science China Press. Published by Elsevier B.V. and Science China Press. All rights reserved. 1806 H. Shen et al. / Science Bulletin 64 (2019) 1805–1816 for electrochemical reduction of CO2. In homogeneous catalysis, revealed that the tailoring of catalytic reaction systems may although many metal complexes [26] and clusters [27] have been change the activity and selectivity of the catalysts and sometimes reported to reduce CO2 to small molecules such as CO with high even reverse their performance trends [57]. Therefore, system selectivity, the high cost and the difficulty of separation have engineering-based research on the full CO2RR, including the pro- greatly limited their value for practical use. In contrast, inorganic cess and device architecture, is equally critical as the catalyst material-based heterogeneous catalysts have attracted more and design in order to attain the goal of future industrial application. more attention from the research community, due to their simplic- In this review, we will summarize recent innovations on the ity of synthesis, environmental friendliness, and high chemical reactor architecture and optimizations based on system engineer- stability in a reductive environment [28]. Both metal-free and ing in the CO2RR (Fig. 1). The improvements of the CO2RR in core metal-based catalysts have shown activity in electrocatalytic metrics of such as the catalytic current density, energy conversion CO2RR. Different product selectivity can be achieved by doping efficiency, and selectivity, will then be discussed based on the reac- non-metallic heteroatoms with various elemental compositions tor design innovation, energy input regulation, as well as electrode and site structures on carbon-based metal-free electrocatalysts structure and electrolyte optimization. These improvements are [29–31]. More heterogeneous catalysts for electrochemical reduc- critical for industrial and commercial applications, and also sug- tion of CO2 are metal-based materials such as Cu, Ag, Au and Sn [32]. gest a guide how to further enhance the performance of CO2RR According to the intermediate states of the catalytic process and from a system engineering perspective. Finally, several critical the main products of the catalytic reaction, the catalysts can be challenges and future trends focusing on the CO2RR system engi- roughly classified into three different categories [33]. The type I neering will be proposed and discussed. electrocatalysts are mainly composed of the main group metal such as Sn, Pb, In, Bi, and Hg, which has a strong binding ability À 2. Catalytic reactor design to the intermediate state CO2* . The reduction process mainly pro- ceeds to an outer layer mechanism, and the main product is formic 2.1. Microfluidic reactor acid or in the form of formate at a basic environment [34–36]. The type II electrocatalysts are generally late transition metal materials Due to the mass transport limitation of CO2 dissolved in the liq- such as Ag, Au, Zn, and Pd, which have strong binding ability to the uid electrolyte, the traditional H-type reactors are subject to a low *COOH intermediate, but their adsorption to the *CO intermediate achievable catalytic current density, which seriously hindered is weak, so the main product is carbon monoxide (CO) [37,38]. Cop- their large-scale application. Gas diffusion electrode (GDE)- per is the only type III of catalyst. It has a strong binding to the assisted microfluidic reactors are pioneered by Kenis and his co- intermediate state *CO and can be further reduced to form a workers in order to solve this problem [58]. In this type of reactors *COH or *CHO intermediate state [39,40]. The products of (Fig. 2a), two GDEs are coated with a catalyst for cathodic CO2RR, copper-based material are abundant and can include hydrocarbons and another catalyst for anodic oxygen evolution reaction (OER) and alcohol molecules with 2–3 carbon atoms [41]. Based on the catalyst, respectively. Two electrolytes are separated by an ion- selectivity of different metals for CO RR products, researchers have 2 exchange membrane and flow between the GDEs. A continuous developed electrocatalysts with high selectivity for the synthesis of flow of CO2 is fed to the back of cathodic catalyst-coated GDE as high value-added compounds such as CO [42], methane (CH ) [43], 4 the reaction substance. The stainless steel plates serve as
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