Developing efficient and durable electrocatalysts for acidic oxygen evolution reaction(OER)is pivotal for advancing proton exchange membrane water electrolysis(PEMWEs),yet balancing activity and stability remains a fo...Developing efficient and durable electrocatalysts for acidic oxygen evolution reaction(OER)is pivotal for advancing proton exchange membrane water electrolysis(PEMWEs),yet balancing activity and stability remains a formidable challenge.Herein,we propose a dual-engineering strategy to stabilize Ru-based catalysts by synergizing the oxygen vacancy site-synergized mechanism-lattice oxygen mechanism(OVSM-LOM)with Ru-N bond stabilization.The engineered RuO_(2)@NCC catalyst exhibits exceptional OER performance in 0.5 M H2SO4,achieving an ultralow overpotential of 215 mV at 10 mA cm^(-2) and prolonged stability for over 327 h.The catalyst delivers 300 h of continuous operation at 1 A cm^(-2),with a negligible degradation rate of only 0.067 mV h-1,further demonstrating its potential for practical application.Oxygen vacancies unlock the OVSM-LOM pathway,bypassing the sluggish adsorbate evolution mechanism(AEM)and accelerating reaction kinetics,while the Ru-N bonds suppress Ru dissolution by anchoring low-valent Ru centers.Quasi-in situ X-ray photoelectron spectroscopy(XPS),X-ray absorption spectroscopy(XAS),and isotopic labeling experiments confirm the lattice oxygen participation with *O formation as the rate-determining step.The Ru-N bonds reinforce the structural integrity by stabilizing low-valent Ru centers and inhibiting overoxidation.Theoretical calculations further verify that the synergistic interaction between OVs and Ru-O(N)active sites optimizes the Ru d-band center and stabilizes intermediates,while Ru-N coordination enhances structural integrity.This study establishes a novel paradigm for designing robust acidic OER catalysts through defect and coordination engineering,bridging the gap between activity and stability for sustainable energy technologies.展开更多
血管内大B细胞淋巴瘤(intravascular large B-cell lymphoma,IVLBCL)是一种罕见且具高度侵袭性的结外非霍奇金淋巴瘤。本文报道1例IVLBCL患者,以中枢神经系统症状起病,诊治过程曲折漫长,曾诊断为中枢神经系统脱髓鞘病变和血管炎,历经糖...血管内大B细胞淋巴瘤(intravascular large B-cell lymphoma,IVLBCL)是一种罕见且具高度侵袭性的结外非霍奇金淋巴瘤。本文报道1例IVLBCL患者,以中枢神经系统症状起病,诊治过程曲折漫长,曾诊断为中枢神经系统脱髓鞘病变和血管炎,历经糖皮质激素及免疫抑制剂治疗失败、先后2次手术病理活检才最终确诊为IVLBCL。确诊后采用大剂量甲氨蝶呤联合R-CHOP方案和R-DHAP方案先后各治疗4个疗程和6个疗程,病灶缩小,症状改善,但神经功能始终未恢复,生活无法自理,目前规律随访中。展开更多
基金support from the National Natural Science Foundation of China(Nos.12305373 and 52276220)the Guangzhou Basic Research Program(No.SL2024A04J00234).
文摘Developing efficient and durable electrocatalysts for acidic oxygen evolution reaction(OER)is pivotal for advancing proton exchange membrane water electrolysis(PEMWEs),yet balancing activity and stability remains a formidable challenge.Herein,we propose a dual-engineering strategy to stabilize Ru-based catalysts by synergizing the oxygen vacancy site-synergized mechanism-lattice oxygen mechanism(OVSM-LOM)with Ru-N bond stabilization.The engineered RuO_(2)@NCC catalyst exhibits exceptional OER performance in 0.5 M H2SO4,achieving an ultralow overpotential of 215 mV at 10 mA cm^(-2) and prolonged stability for over 327 h.The catalyst delivers 300 h of continuous operation at 1 A cm^(-2),with a negligible degradation rate of only 0.067 mV h-1,further demonstrating its potential for practical application.Oxygen vacancies unlock the OVSM-LOM pathway,bypassing the sluggish adsorbate evolution mechanism(AEM)and accelerating reaction kinetics,while the Ru-N bonds suppress Ru dissolution by anchoring low-valent Ru centers.Quasi-in situ X-ray photoelectron spectroscopy(XPS),X-ray absorption spectroscopy(XAS),and isotopic labeling experiments confirm the lattice oxygen participation with *O formation as the rate-determining step.The Ru-N bonds reinforce the structural integrity by stabilizing low-valent Ru centers and inhibiting overoxidation.Theoretical calculations further verify that the synergistic interaction between OVs and Ru-O(N)active sites optimizes the Ru d-band center and stabilizes intermediates,while Ru-N coordination enhances structural integrity.This study establishes a novel paradigm for designing robust acidic OER catalysts through defect and coordination engineering,bridging the gap between activity and stability for sustainable energy technologies.
文摘血管内大B细胞淋巴瘤(intravascular large B-cell lymphoma,IVLBCL)是一种罕见且具高度侵袭性的结外非霍奇金淋巴瘤。本文报道1例IVLBCL患者,以中枢神经系统症状起病,诊治过程曲折漫长,曾诊断为中枢神经系统脱髓鞘病变和血管炎,历经糖皮质激素及免疫抑制剂治疗失败、先后2次手术病理活检才最终确诊为IVLBCL。确诊后采用大剂量甲氨蝶呤联合R-CHOP方案和R-DHAP方案先后各治疗4个疗程和6个疗程,病灶缩小,症状改善,但神经功能始终未恢复,生活无法自理,目前规律随访中。
