This paper presented a novel and environmentally friendly approach for recovering platinum group metals(PGMs)from spent automotive exhaust catalysts.The study employed lead slag and waste graphite electrodes as raw ma...This paper presented a novel and environmentally friendly approach for recovering platinum group metals(PGMs)from spent automotive exhaust catalysts.The study employed lead slag and waste graphite electrodes as raw materials,incorporating CaO as an additive to fine-tune the slag's viscosity and density.By reducing FeO in the lead slag using waste graphite electrodes,pure Fe was obtained,effectively trapping the PGMs from the exhausted catalysts.The study explored the effects of reductant addition,trapping duration,slag basicity,and trapping temperature on the recovery rate of PGMs.The results indicated that a maximum recovery rate of 97.86%was achieved when the reductant was added at 1.5 times the theoretical amount,with a trapping duration of 60 minutes,a slag basicity of 0.7,and a trapping temperature of 1600℃.This research offered a greener pathway for the recovery of PGMs from spent automotive exhaust catalysts.展开更多
铂族金属(Platinum Group Metals,PGMs)是我国关键战略资源。其回收利用备受关注。铁捕集法作为主流火法工艺,所获Fe-PGMs合金结构致密、化学惰性强,难以破碎处理,制约后续富集与提纯。湿法工艺在处理此类合金时面临诸多挑战,如酸耗量...铂族金属(Platinum Group Metals,PGMs)是我国关键战略资源。其回收利用备受关注。铁捕集法作为主流火法工艺,所获Fe-PGMs合金结构致密、化学惰性强,难以破碎处理,制约后续富集与提纯。湿法工艺在处理此类合金时面临诸多挑战,如酸耗量大、生产成本高以及环境污染严重等。因此,如何从Fe-PGMs合金分离出PGMs成为解决问题的关键。综述了Fe-PGMs合金在富集前预处理阶段的工艺技术现状,评估了各工艺的优缺点。展开更多
Perfect anomalous reflections have been demonstrated in optical phase gradient metasurfaces(PGMs),but they suffer from single-frequency(narrow-band)response due to the intrinsic limitation of natural geometric periodi...Perfect anomalous reflections have been demonstrated in optical phase gradient metasurfaces(PGMs),but they suffer from single-frequency(narrow-band)response due to the intrinsic limitation of natural geometric periodicity.Here,we provide both numerical and analytical evidence that a depth gradient metasurface can achieve discrete ultra-broadband perfect anomalous reflection in the microwave range in the absence of geometric periodicity.Remarkably,by adjusting the operating frequency of the incident wave,the same effect can be steadily obtained via a physically equivalent phase periodicity in the PGM.Based on this mechanism,a perfect retroreflector with a broadband response ranging from 1 GHz to 40 GHz is realized.Our work has promising applications in communication,source tracking,and military satellites.展开更多
Fe-N-doped carbon materials(Fe-N-C)are promising candidates for oxygen reduction reaction(ORR)relative to Pt-based catalysts in proton exchange membrane fuel cells(PEMFCs).However,the intrinsic contributions of Fe-N_(...Fe-N-doped carbon materials(Fe-N-C)are promising candidates for oxygen reduction reaction(ORR)relative to Pt-based catalysts in proton exchange membrane fuel cells(PEMFCs).However,the intrinsic contributions of Fe-N_(4)moiety with different chemical/spin states(e.g.D1,D2,D3)to ORR are unclear since various states coexist inevitably.In the present work,Fe-N-C core-shell nanocatalyst with single lowspin Fe(Ⅱ)-N_(4)species(D1)is synthesized and identified with ex-situ ultralow temperature Mossbauer spectroscopy(T=1.6 K)that could essentially differentiate various Fe-N_(4)states and invisible Fe-O species.By quantifying with CO-pulse chemisorption,site density and turnover frequency of Fe-N-C catalysts reach 2.4×10^(-9)site g^(-1)and 23 e site~(-1)s^(-1)during the ORR,respectively.Half-wave potential(0.915V_(RHE))of the Fe-N-C catalyst is more positive(approximately 54 mV)than that of Pt/C.Moreover,we observe that the performance of PEMFCs on Fe-N-C almost achieves the 2025 target of the US Department of Energy by demonstrating a current density of 1.037 A cm^(-2)combined with the peak power density of 0,685 W cm^(-2),suggesting the critical role of Fe(Ⅱ)-N_(4)site(D1).After 500 h of running,PEMFCs still deliver a power density of 1.26 W cm^(-2)at 1.0 bar H_(2)-O_(2),An unexpected rate-determining step is figured out by isotopic labelling experiment and theoretical calculation.This work not only offers valuable insights regarding the intrinsic contribution of Fe-N_(4)with a single spin state to alkaline/acidic ORR,but also provides great opportunities for developing high-performance stable PEMFCs.展开更多
基金Funded by the Natural Science Foundation of Henan(No.252300421563)the Key Research Projects of Henan Provincial Colleges and Universities(No.25B450001)+3 种基金the Basic and Frontier Research Project of Nanyang(No.24JCQY032)National Natural Science Foundation of China(No.52201044)the Key Specialized Research&Development and Promotion Project(Scientific and Technological Project)of Henan Province(No.232102221022)the Basic and Frontier Technology Research Project of Nanyang(No.23JCQY1001)。
文摘This paper presented a novel and environmentally friendly approach for recovering platinum group metals(PGMs)from spent automotive exhaust catalysts.The study employed lead slag and waste graphite electrodes as raw materials,incorporating CaO as an additive to fine-tune the slag's viscosity and density.By reducing FeO in the lead slag using waste graphite electrodes,pure Fe was obtained,effectively trapping the PGMs from the exhausted catalysts.The study explored the effects of reductant addition,trapping duration,slag basicity,and trapping temperature on the recovery rate of PGMs.The results indicated that a maximum recovery rate of 97.86%was achieved when the reductant was added at 1.5 times the theoretical amount,with a trapping duration of 60 minutes,a slag basicity of 0.7,and a trapping temperature of 1600℃.This research offered a greener pathway for the recovery of PGMs from spent automotive exhaust catalysts.
文摘铂族金属(Platinum Group Metals,PGMs)是我国关键战略资源。其回收利用备受关注。铁捕集法作为主流火法工艺,所获Fe-PGMs合金结构致密、化学惰性强,难以破碎处理,制约后续富集与提纯。湿法工艺在处理此类合金时面临诸多挑战,如酸耗量大、生产成本高以及环境污染严重等。因此,如何从Fe-PGMs合金分离出PGMs成为解决问题的关键。综述了Fe-PGMs合金在富集前预处理阶段的工艺技术现状,评估了各工艺的优缺点。
基金supported by the National Natural Science Foundation of China(Grant Nos.12274313,62275184,and 62411540033)Collaborative Innovation Center of Suzhou Nano Science and Technology,Suzhou Basic Research Project(Grant No.SJC2023003)+1 种基金the Gusu Leading Talent Plan for Scientific and Technological Innovation and Entrepreneurship(Grant No.ZXL2024400)the Priority Academic Program Development of Jiangsu Higher Education Institutions.
文摘Perfect anomalous reflections have been demonstrated in optical phase gradient metasurfaces(PGMs),but they suffer from single-frequency(narrow-band)response due to the intrinsic limitation of natural geometric periodicity.Here,we provide both numerical and analytical evidence that a depth gradient metasurface can achieve discrete ultra-broadband perfect anomalous reflection in the microwave range in the absence of geometric periodicity.Remarkably,by adjusting the operating frequency of the incident wave,the same effect can be steadily obtained via a physically equivalent phase periodicity in the PGM.Based on this mechanism,a perfect retroreflector with a broadband response ranging from 1 GHz to 40 GHz is realized.Our work has promising applications in communication,source tracking,and military satellites.
基金financial support from the“Hundred Talents Program”of the Chinese Academy of Sciencesthe“Young Talents Training Program”of the Shanghai Branch of the Chinese Academy of Sciences+3 种基金the financial support from the Xiamen City Natural Science Foundation of China(3502Z20227085,3502Z20227256)the National Science Youth Foundation of China(22202205)the Fujian Provincial Natural Science Foundation of China(2022J01502)Open Source Foundation of State Key Laboratory of Structural Chemistry。
文摘Fe-N-doped carbon materials(Fe-N-C)are promising candidates for oxygen reduction reaction(ORR)relative to Pt-based catalysts in proton exchange membrane fuel cells(PEMFCs).However,the intrinsic contributions of Fe-N_(4)moiety with different chemical/spin states(e.g.D1,D2,D3)to ORR are unclear since various states coexist inevitably.In the present work,Fe-N-C core-shell nanocatalyst with single lowspin Fe(Ⅱ)-N_(4)species(D1)is synthesized and identified with ex-situ ultralow temperature Mossbauer spectroscopy(T=1.6 K)that could essentially differentiate various Fe-N_(4)states and invisible Fe-O species.By quantifying with CO-pulse chemisorption,site density and turnover frequency of Fe-N-C catalysts reach 2.4×10^(-9)site g^(-1)and 23 e site~(-1)s^(-1)during the ORR,respectively.Half-wave potential(0.915V_(RHE))of the Fe-N-C catalyst is more positive(approximately 54 mV)than that of Pt/C.Moreover,we observe that the performance of PEMFCs on Fe-N-C almost achieves the 2025 target of the US Department of Energy by demonstrating a current density of 1.037 A cm^(-2)combined with the peak power density of 0,685 W cm^(-2),suggesting the critical role of Fe(Ⅱ)-N_(4)site(D1).After 500 h of running,PEMFCs still deliver a power density of 1.26 W cm^(-2)at 1.0 bar H_(2)-O_(2),An unexpected rate-determining step is figured out by isotopic labelling experiment and theoretical calculation.This work not only offers valuable insights regarding the intrinsic contribution of Fe-N_(4)with a single spin state to alkaline/acidic ORR,but also provides great opportunities for developing high-performance stable PEMFCs.
