Efficient Electrosynthesis of Syngas with Tunable CO/H₂Ratios over Zn_xCd_1−xS‐Amine Inorganic–Organic Hybrids

Abstract

Efficient electrochemical reduction of CO2 and H2O into industrial syngas with tunable CO/H2 ratios, especially integrated with anodic organic synthesis to replace the low‐value oxygen evolution reaction (OER), is highly desirable. Here, integration of controllable partial substitution of zinc (Zn) with amine incorporation into CdS‐amine inorganic‐organic hybrids is used to generate highly efficient electrocatalysts for synthesizing syngas with tunable CO/H2 ratios (0–19.7), which are important feedstocks for the Fischer–Tropsch process. Diethylenetriamine could enhance the adsorption and accelerate the activation of CO2 to form the key intermediate COOH* for CO formation. Zn substitution promoted the hydrogen evolution reaction (HER), leading to tunable CO/H2 ratios. Importantly, syngas and dihydroisoquinoline can be simultaneously synthesized by pairing with anodic semi‐oxidation of tetrahydroisoquinoline in a ZnxCd1−xS‐Amine ∥ Ni2P two‐electrode electrolyzer.

Ru‐Pincer Complex‐Bridged Cu‐Porphyrin Polymer for Robust (Photo)Electrocatalytic H2 Evolution via Single‐Atom Active Sites

“…To get fundamental insight into the intrinsic activity, the electrochemical active surface areas (ECSA) of those polymers were assessed by measuring the electrochemical layer capacitance (C dl ) due to their positive proportion relationship (Figure S27, Supporting Information). [44,45] As depicted in Figure 3e, the ECSA (37.8 cm 2 ) of metal-free H 2 Por-N 3 is much smaller than that of CuPor-N 3 (42.8 cm 2 ), H 2 Por-RuN 3 (75.0 cm 2 ) and CuPor-RuN 3 (72.2 cm 2 ), demonstrating that the introduction of metal centers is beneficial for exposing more active sites. From the LSV curves (Figure 3f) after being ECSA-normalized, it can be found that CuPor-RuN 3 still shows an intrinsic electrocatalytic activity superior to H 2 Por-N 3 , CuPor-N 3 and H 2 Por-RuN 3 , demonstrating that the Cu/Ru hetero-bimetallic centers induce the well-suited electronic structure and improve the reactivity of single-atom active sites.…”

Highly Efficient Photoreduction of Low‐Concentration CO2to Syngas by Using a Polyoxometalates/RuIIComposite

“…Syngas, composedo fH 2 and CO, is as ignificant feedstock for production of high-valued longerh ydrocarbons through wellestablished processes, such as the Fischer-Tropsch (F-T) process and syngas fermentation. [1,2] CO 2 photoreduction driven by sunlight not only provides an alternate approach for the generation of useful chemicals (e.g.,s yngas) in an environmentally friendly, [3][4][5] sustainable, and low-cost way but also alleviates the environmental burden caused by excessive CO 2 emissions. Numerous photocatalysts with high activity have been developedf or CO 2 reduction to syngas, but they usually use pure CO 2 ,w hich needs to be extracted from the atmosphere first.…”

Plasma-regulated N-doped carbon nanotube arrays for efficient electrosynthesis of syngas with a wide CO/H2 ratio

“…The band at 1635 cm −1 is attributed to interfacial water [44]. While the band at 1400 cm −1 represents the absorption of *COOH [45,46], indicating the formation of CO is with *COOH as the intermediate. The *COOH intensity of pCNTA10 is slightly stronger than that of CNTA, reflecting that the plasma treatment is beneficial to the selectivity to CO.…”