Pal Santanu, Sinha Nibedita, Das Chandni, Chauhan Inderjeet, Ahmed Tanbir, Roy Poulomi
CSIR─Central Mechanical Engineering Research Institute (CMERI), Durgapur 713209, West Bengal, India.
Physical and Materials Chemistry Division, CSIR─National Chemical Laboratory (NCL), Pune 411008, Maharashtra, India.
ACS Appl Mater Interfaces. 2025 Jul 2;17(26):37863-37878. doi: 10.1021/acsami.5c04189. Epub 2025 Jun 16.
Layered double hydroxides (LDHs) have attracted much attention these days in the field of water electrolysis due to easy modulation in their layered structure and properties. Herein, NiCr-LDH has been developed, and its interlayer spacing has been considerably increased by oxalate intercalation. Such increased interlayer spacing allows easy access of hydroxides to a large number of electroactive sites and thereby boosts the electrocatalytic performances both for oxygen and hydrogen evolution reactions. Being very active toward both the electrocatalytic reactions, the oxalate-intercalated NiCr-LDH was further explored in an alkaline anion exchange membrane water electrolyzer (AEMWE), achieving 800 mA cm at 1.88 V cell voltage at an operating temperature of 60 °C. In fact, the electrolyzer efficiency has been determined to be as high as 69.66%, and the calculated H production cost was found to be $0.97 per gasoline-gallon equivalent, which is well below the targeted cost by the Department of Energy, USA. The electrocatalyst was also examined in harsh alkaline media, like highly saline or seawater, which also indicated its ability to carry out sustainable seawater electrolysis, restricting chlorides to a great extent. Interestingly, post-electrolysis characterization reveals the fact that oxalate decomposition aided carbonate formation within interlayers of NiCr-LDH, and high affinity toward hydroxides is responsible for restricting chlorides during the electrolysis process, apart from the great electrocatalytic activity.
层状双氢氧化物(LDHs)近来因其层状结构和性质易于调控而在水电解领域备受关注。在此,已开发出NiCr-LDH,其层间距通过草酸盐插层得到显著增加。这种增加的层间距使氢氧化物易于接近大量电活性位点,从而提高了析氧和析氢反应的电催化性能。由于对两种电催化反应都非常活跃,草酸盐插层的NiCr-LDH在碱性阴离子交换膜水电解槽(AEMWE)中得到进一步研究,在60℃的操作温度下,在1.88V的电池电压下实现了800mA/cm²的电流密度。实际上,已确定该电解槽效率高达69.66%,计算得出的每加仑汽油当量的制氢成本为0.97美元,这远低于美国能源部设定的目标成本。该电催化剂还在高盐或海水等苛刻的碱性介质中进行了测试,这也表明其能够进行可持续的海水电解,在很大程度上限制了氯化物的影响。有趣的是,电解后表征揭示了这样一个事实,即草酸盐分解有助于在NiCr-LDH层间形成碳酸盐,并且除了具有很高的电催化活性外,对氢氧化物的高亲和力也是在电解过程中限制氯化物的原因。