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Electrochemical Biomass Upgrading Coupled with Hydrogen Production under Industrial-Level Current Density
Advanced Materials ( IF 27.4 ) Pub Date : 2023-03-25 , DOI: 10.1002/adma.202300935 Qizhu Qian 1 , Xiaoyue He 1 , Ziyun Li 1 , Yanxu Chen 1 , Yafei Feng 1 , Mingyu Cheng 1 , Huaikun Zhang 1 , Wentao Wang 2 , Chong Xiao 1, 3 , Genqiang Zhang 1 , Yi Xie 1, 3
Advanced Materials ( IF 27.4 ) Pub Date : 2023-03-25 , DOI: 10.1002/adma.202300935 Qizhu Qian 1 , Xiaoyue He 1 , Ziyun Li 1 , Yanxu Chen 1 , Yafei Feng 1 , Mingyu Cheng 1 , Huaikun Zhang 1 , Wentao Wang 2 , Chong Xiao 1, 3 , Genqiang Zhang 1 , Yi Xie 1, 3
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As promising hydrogen energy carrier, formic acid (HCOOH) plays an indispensable role in building a complete industry chain of a hydrogen economy. Currently, the biomass upgrading assisted water electrolysis has emerged as an attractive alternative for co-producing green HCOOH and H2 in a cost-effective manner, yet simultaneously affording high current density and Faradaic efficiency (FE) still remains a big challenge. Here, the ternary NiVRu-layered double hydroxides (LDHs) nanosheet arrays for selective glycerol oxidation and hydrogen evolution catalysis are reported, which yield an industry-level 1 A cm−2 at voltage of 1.933 V, meanwhile showing considerable HCOOH and H2 productivities of 12.5 and 17.9 mmol cm−2 h−1, with FEs of almost 80% and 96%, respectively. Experimental and theoretical results reveal that the introduced Ru atoms can tune the local electronic structure of Ni-based LDHs, which not only optimizes hydrogen adsorption kinetics for HER, but also reduces the reaction energy barriers for both the conversion of NiII into GOR-active NiIII and carboncarbon (CC) bond cleavage. In short, this work highlights the potential of large-scale H2 and HCOOH productions from integrated electrocatalytic system and provides new insights for designing advanced electrocatalyst for low-cost and sustainable energy conversion.
中文翻译：
工业级电流密度下电化学生物质升级联产氢
甲酸（HCOOH）作为极具前景的氢能源载体，在构建氢经济完整产业链中发挥着不可或缺的作用。目前，生物质升级辅助水电解已成为一种具有成本效益的联产绿色HCOOH和H 2的有吸引力的替代方案，但同时提供高电流密度和法拉第效率（FE）仍然是一个巨大的挑战。在此，报道了用于选择性甘油氧化和析氢催化的三元NiVRu层状双氢氧化物（LDH）纳米片阵列，其在1.933 V的电压下产生工业水平的1 A cm -2 ，同时显示出相当大的HCOOH和H 2生产率12.5 和 17.9 mmol cm -2 h -1，FE 分别接近 80% 和 96%。实验和理论结果表明，引入的Ru原子可以调节Ni基LDH的局域电子结构，这不仅优化了HER的氢吸附动力学，而且降低了Ni II转化为GOR活性的反应能垒NiⅢ与碳碳(CC )键断裂。简而言之，这项工作凸显了集成电催化系统大规模生产H 2和HCOOH的潜力，并为设计用于低成本和可持续能源转换的先进电催化剂提供了新的见解。
更新日期：2023-03-25
中文翻译：
工业级电流密度下电化学生物质升级联产氢
甲酸（HCOOH）作为极具前景的氢能源载体，在构建氢经济完整产业链中发挥着不可或缺的作用。目前，生物质升级辅助水电解已成为一种具有成本效益的联产绿色HCOOH和H 2的有吸引力的替代方案，但同时提供高电流密度和法拉第效率（FE）仍然是一个巨大的挑战。在此，报道了用于选择性甘油氧化和析氢催化的三元NiVRu层状双氢氧化物（LDH）纳米片阵列，其在1.933 V的电压下产生工业水平的1 A cm -2 ，同时显示出相当大的HCOOH和H 2生产率12.5 和 17.9 mmol cm -2 h -1，FE 分别接近 80% 和 96%。实验和理论结果表明，引入的Ru原子可以调节Ni基LDH的局域电子结构，这不仅优化了HER的氢吸附动力学，而且降低了Ni II转化为GOR活性的反应能垒NiⅢ与碳碳(CC )键断裂。简而言之，这项工作凸显了集成电催化系统大规模生产H 2和HCOOH的潜力，并为设计用于低成本和可持续能源转换的先进电催化剂提供了新的见解。
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