Proton exchange membrane electrolysis of methanol for simultaneously synthesizing formaldehyde and hydrogen
Proton exchange membrane electrolysis of methanol for simultaneously synthesizing formaldehyde and hydrogen
复制标题
质子交换膜电解甲醇同时合成甲醛和氢气
DOI：
10.1039/d2se01472f
复制
发表时间：
2023
影响因子：
5.6
通讯作者：
Kurokawa Hideki
中科院分区：
文献类型：
--
作者：
Kuramochi Nanako;Yoshida-Hirahara Miru;Ogihara Hitoshi;Kurokawa Hideki
用于升级分子的电解作为可以有助于可持续社会的绿色过程而受到关注。在这项研究中，甲醇（MeOH）转化为甲醛（FA）和H2通过电解使用膜电极组件（MEA）装置，其中Nafion被用作质子交换膜（PEM）。比较PEM电解的各种阳极催化剂，发现Pd/C以高法拉第效率（CH 3OH → HCHO +2 H + +2 e −）产生FA。Pd负载量和电解电压影响FA的生成速率。在PEM电解中，形成的质子通过Nafion膜向阴极移动，并且在阴极上放出H2（2 H ++2e − → H2），这表明该电解系统同时产生FA和H2。通过FA和MeOH的非电化学缩醛化形成副产物二甲氧基甲烷（DMM），其中Nafion用作酸催化剂。通过搅拌电解液和加入少量水来抑制DMM的形成。在这项研究中的FA形成速率（682 mmol gcat−1 h−1）超过了先前研究中报道的那些，其中FA是通过多相催化和光催化系统从MeOH脱氢合成的。
Electrolysis for upgrading molecules has received attention as a green process that can contribute to a sustainable society. In this study, methanol (MeOH) was converted into formaldehyde (FA) and H2via electrolysis using a membrane electrode assembly (MEA) device, wherein Nafion was used as a proton exchange membrane (PEM). Comparing various anode catalysts for PEM electrolysis, Pd/C is found to produce FA at a high faradaic efficiency (CH3OH → HCHO + 2H+ + 2e−). Pd loading and electrolysis voltage affect the FA formation rate. In the PEM electrolysis, the formed protons move toward the cathode through the Nafion membrane, and H2 is evolved on the cathode (2H+ + 2e− → H2), which indicates that this electrolysis system simultaneously yields FA and H2. A by-product, dimethoxymethane (DMM), is formed through the non-electrochemical acetalization of FA and MeOH, where Nafion serves as an acid catalyst. The formation of DMM is inhibited by stirring the electrolysis solution and adding a small amount of water. The FA formation rate (682 mmol gcat−1 h−1) in this study exceeds those reported in previous studies wherein FA is synthesized from the dehydrogenation of MeOH via heterogeneous catalytic and photocatalytic systems.