Molecular single iron site catalysts for electrochemical nitrogen fixation under ambient conditions

Boosting Electroreduction Kinetics of Nitrogen to Ammonia via Tuning Electron Distribution of Single‐Atomic Iron Sites

“…To confirm the reliability, 15 N 2 (99 atom% 15 N) isotope labeling experiments were performed on Fe SA -NO-C-900. As shown in Figure 4e,dominant peaks of doublet coupling for 15 NH 4 + and triplet coupling for 14 NH 4 + ,r espectively,w ere seen on the 1 HNMR spectra in the case of using 15 N 2 and 14 N 2 ,r espectively,a st he feeding gas,i ndicating that the N 2 feeding gas was the sole source for the formation of NH 3 from the electrocatalytic NRR. Thee lectrocatalytic stability of Fe SA -NO-C-900 towards NRR was also investigated by cycling and chronoamperometric measurements at À0.4 Vb yr eplacing the electrolyte every 2h.A ss hown in Figure 4f,n oo bvious change in both the NH 3 production rate and FE NH3 was observed during 10 consecutive cycles,suggesting an excellent stability for Fe SA -NO-C-900.…”

Progress in Mo/W-based electrocatalysts for nitrogen reduction to ammonia under ambient conditions

“…6(f)). 37 This constructed 2D/2D MoS 2 /C 3 N 4 heterojunction could essentially prevent HER behaviors and promote the e-NRR activity with a high FE of 17.8% at À0.3 V vs. RHE, contributing to the formation of the coupling interaction effect between MoS 2 and C 3 N 4 . Furthermore, to prevent the aggregation of the materials, Thoi et al designed a highly dispersed MoO 2 NPs/carbon catalyst (carbon nanowire serving as support, as displayed in Fig.…”

“…32,33 Remarkably, in addition to the common neutral electrolyte, Mo/W-based catalysts also showed admirable catalytic activity and stability in alkaline 18 and acidic conditions. 15 Until now, to further overcome the bottleneck and the completing hydrogen evolution reaction (HER), much research work has been devoted to developing high-performance e-NRR electrocatalysts through various strategies, including morphology regulation, 34,35 vacancy creation, 36 defect-rich surface tailoring, 11 crystal structure optimization, 26 interface engineering, 37,38 reactive cell design, 39 etc. However, to the best of our knowledge, a specific review focused on advances in the Mo/W catalysts for the NRR has not been reported.…”

Porphyrin and phthalocyanine: from molecular materials to aggregates

“…ZnTCPP/THPP 双卟啉异质催化剂在光催化析氢反应 中表现出优异的性能(图 8a) [124] 。并且有大量的理 论计算都已经证明了，卟啉酞菁类物质，对电催化 [128] 。在这项研究中，对卟啉配体进 行给电子或吸电子取代基修饰对平衡过电位(η) 和电子驱动力 Edf 以实现光催化水氧化性能优化的重 要作用得以揭示。 卟啉、酞菁分子具有共轭、极性、高度离域的 分子特性以及稳定的金属配位环境。上述特点使得 卟啉、酞菁在电催化领域极具发展潜力 [142] 。但导电 性低，本征催化活性不佳等问题限制了卟啉、酞菁 催化剂的应用。为解决这些问题，科学家通过促进 电荷转移、调整活性位点配位环境、官能团修饰等 策略使得卟啉、酞菁作为一类高效的电催化剂在电 化学氧还原反应(ORR) [26,[143][144][145] 、电化学分解水析 氢(HER) [146][147][148][149][150] 、电化学水氧化(OER) [23,146,151,152] 、电化学 CO2 还原反应(CO2RR) [153][154][155][156][157][158][159] 、电化 学氮还原反应(NRR) [21,24,[160][161][162] 中表现突出。对于 电催化反应，卟啉、酞菁常常与碳材料相结合来降 低团聚现象并使得异质催化剂获得更为优异的导电 性。据报道，钴酞菁(CoPc)可以通过非共价键锚 定于石墨炔/石墨烯(GDY/G)支架以用于电催化…”