The global shift toward carbon neutrality,driven by growing concerns about climate change,requires collaborative efforts.While cleaner energy and carbon capture are crucial,addressing some high-carbon-emission industr...The global shift toward carbon neutrality,driven by growing concerns about climate change,requires collaborative efforts.While cleaner energy and carbon capture are crucial,addressing some high-carbon-emission industrial processes that significantly and disproportionally contribute to our carbon footprint is more important than ever.Analysis reveals that over 90%of total carbon emissions from human activities are attributed to a few super-emitting thermochemical processes.We urgently need breakthrough technologies and transformative alternatives to combat this excess of carbon dioxide emissions effectively.Engineering Thermochemistry is the scientific discipline that offers both scientifically sound and practical solutions to the pressing carbon neutrality challenges.展开更多
为了利用X射线吸收精细结构(X-ray absorption fine structure,XAFS)谱学技术开展热化学反应动力学研究,在上海光源X射线吸收精细结构谱学线站(BL14W1)开展了时间分辨热化学原位XAFS方法的研究。采用自主研制的数据采集设备解决了时间分...为了利用X射线吸收精细结构(X-ray absorption fine structure,XAFS)谱学技术开展热化学反应动力学研究,在上海光源X射线吸收精细结构谱学线站(BL14W1)开展了时间分辨热化学原位XAFS方法的研究。采用自主研制的数据采集设备解决了时间分辨XAFS技术中不同类型信号同步触发和同步采集的问题,实现了数据间的精准匹配。在单色器转速为720"/s、数据采集设备采样率为2MS/s、数据长度为1200eV的条件下,获得了一个9.6s的Cu标样的数据谱,通过与常规XAFS数据和标准XAFS数据进行对比,结果表明本文得到的时间分辨XAFS实验系统具有良好的准确性、分辨率和信噪比。在此基础上,进一步结合线站自主研制的原位装置开展了时间分辨热化学原位XAFS方法,并利用高温常压原位装置开展了CuO还原为金属Cu的验证性实验。在230℃恒温氢气气氛下30min内观测到Cu吸收边能量逐渐向低能量处偏移,同时它位于8998eV的主峰强度逐渐减弱并且劈裂为双峰结构,出现明显的金属Cu的特征。实验结果表明此方法达到了捕获物质动态演化过程的预期目的,在拓展XAFS谱学实验平台的同时,为热化学反应的动力学过程研究提供了一种强大的实验手段。展开更多
The climate crisis necessitates the development of non-fossil energy sources.Harnessing solar energy for fuel production shows promise and offers the potential to utilize existing energy infrastructure.However,solar f...The climate crisis necessitates the development of non-fossil energy sources.Harnessing solar energy for fuel production shows promise and offers the potential to utilize existing energy infrastructure.However,solar fuel production is in its early stages of development,constrained by low conversion efficiency and challenges in scaling up production.Concentrated solar energy(CSE)technology has matured alongside the rapid growth of solar thermal power plants.This review provides an overview of current CSE methods and solar fuel production,analyzes their integration compatibility,and delves into the theoretical mechanisms by which CSE impacts solar energy conversion efficiency and product selectivity in the context of photo-electrochemistry,thermochemistry,and photo-thermal co-catalysis for solar fuel production.The review also summarizes approaches to studying the photoelectric and photothermal effects of CSE.Lastly,it explores emerging novel CSE technology methods in the field of solar fuel production.展开更多
The complex of samaric chloride lower hydrate with diethylammoniumdiethyldithiocarbamate (D-DDC) was synthesized conveniently in absolute alcohol and dry N_2atmosphere. The title complex was identified as Et_2NH_2[Sm(...The complex of samaric chloride lower hydrate with diethylammoniumdiethyldithiocarbamate (D-DDC) was synthesized conveniently in absolute alcohol and dry N_2atmosphere. The title complex was identified as Et_2NH_2[Sm(S_2CNEt_2)_4] by chemical and elementalanalyses, the bonding characteristics of which was characterized by IR. The enthalpies of solutionof samaric chloride hydrate and D-DDC in absolute alcohol at 298.15 K and the enthalpies change ofliquid-phase reaction of formation for Et_2NH_2[Sm(S_2CNEt_2)_4] at different temperatures weredetermined by mi-crocalorimetry. On the basis of experimental and calculated results, threethermodynamic parameters (the activation enthalpy, the activation entropy, and the activation freeenergy), the rate constant, and three kinetic parameters (the apparent activation energy, thepre-exponential constant, and the reaction order) of liquid phase reaction of formation wereobtained. The enthalpy change of the solid-phase title reaction at 298.15 K was calculated by athermochemical cycle.展开更多
The complex of neodymium chloride lower hydrate with diethylammonium diethyldithiocarbamate (D-DDC) was synthesized conveniently in absolute alcohol and dry N_2 atmosphere. The title complex was identified as Et_2NH_2...The complex of neodymium chloride lower hydrate with diethylammonium diethyldithiocarbamate (D-DDC) was synthesized conveniently in absolute alcohol and dry N_2 atmosphere. The title complex was identified as Et_2NH_2[Nd(S_2CNEt_2)_4] by chemical and elemental analyses and the bonding characteristics of which was characterized by IR. The enthalpies of solution of neodymium chloride hydrate and D-DDC in absolute alcohol at 298.15 K and the enthalpies change of liquid-phase reaction of formation for Et_2NH_2[Nd (S_2CNEt_2)_4] at different temperatures were determined by microcalorimetry. On the basis of experimental and calculated results, three thermodynamic parameters (the activation enthalpy, the activation entropy and the activation free energy), the rate constant and three kinetic parameters (the apparent activation energy, the pre-exponential constant and the reaction order) of liquid-phase reaction of formation were obtained. The enthalpy change of the solid-phase title reaction at 298.15 K was calculated by a thermochemical cycle.展开更多
This paper investigated on influence of different alloying elements added into duplex stainless steel (DSS) on phase transitions using thermochemical methods in comparison with experiment.The results showed that the m...This paper investigated on influence of different alloying elements added into duplex stainless steel (DSS) on phase transitions using thermochemical methods in comparison with experiment.The results showed that the most possible species in the ferrite phase,austenite phase,σphase,Hcp phase,χphase,and carbide were Cr:Va-type,Fe:Va-type,Ni:Cr:Mo-type,Cr_(2)N-type,Fe_(24)Mo_(10)Cr_(24)-type,and Cr:Mo:C-type,respectively.Furthermore,the Ni,N,Cr,and Mo alloying had significant influences on the transition of each DSS phase.The Ni and N additions obviously raised the temperature at ferrite-1/austenite-1 balance while the Cr and Mo decreased the dual-phase balance temperature.In addition,the Ni addition can promote the precipitating ofσphase at relatively high temperature while the precipitating of Hcp phase at relatively low temperature.The Hcp phase andχphase can be obviously increased by the N addition.The introduction of Cr and Mo notably enhances the precipitation ofσphase.However,the promotion ofχphase precipitation is facilitated by the presence of Mo,while the Cr element acts as an inhibitor forχphase precipitation.Furthermore,the ferrite/austenite ratio tested by experiment was higher than that calculated by thermochemical methods,thus pre-designed solution temperature should be lower about 30-100℃than that calculated by thermochemical methods.展开更多
基金partially supported by the National Natural Science Foundation of China(U22A20410).
文摘The global shift toward carbon neutrality,driven by growing concerns about climate change,requires collaborative efforts.While cleaner energy and carbon capture are crucial,addressing some high-carbon-emission industrial processes that significantly and disproportionally contribute to our carbon footprint is more important than ever.Analysis reveals that over 90%of total carbon emissions from human activities are attributed to a few super-emitting thermochemical processes.We urgently need breakthrough technologies and transformative alternatives to combat this excess of carbon dioxide emissions effectively.Engineering Thermochemistry is the scientific discipline that offers both scientifically sound and practical solutions to the pressing carbon neutrality challenges.
文摘为了利用X射线吸收精细结构(X-ray absorption fine structure,XAFS)谱学技术开展热化学反应动力学研究,在上海光源X射线吸收精细结构谱学线站(BL14W1)开展了时间分辨热化学原位XAFS方法的研究。采用自主研制的数据采集设备解决了时间分辨XAFS技术中不同类型信号同步触发和同步采集的问题,实现了数据间的精准匹配。在单色器转速为720"/s、数据采集设备采样率为2MS/s、数据长度为1200eV的条件下,获得了一个9.6s的Cu标样的数据谱,通过与常规XAFS数据和标准XAFS数据进行对比,结果表明本文得到的时间分辨XAFS实验系统具有良好的准确性、分辨率和信噪比。在此基础上,进一步结合线站自主研制的原位装置开展了时间分辨热化学原位XAFS方法,并利用高温常压原位装置开展了CuO还原为金属Cu的验证性实验。在230℃恒温氢气气氛下30min内观测到Cu吸收边能量逐渐向低能量处偏移,同时它位于8998eV的主峰强度逐渐减弱并且劈裂为双峰结构,出现明显的金属Cu的特征。实验结果表明此方法达到了捕获物质动态演化过程的预期目的,在拓展XAFS谱学实验平台的同时,为热化学反应的动力学过程研究提供了一种强大的实验手段。
基金support by the National Key Research and Development Program of China(2022YFB3803600)the National Natural Science Foundation of China(No.52276212)+3 种基金the Natural Science Foundation of Jiangsu Province(No.BK20231211)the Suzhou Science and Technology Program(SYG202101)the Key Research and Development Program in Shaanxi Province of China(No.2023-YBGY-300)the China Fundamental Research Funds for the Central Universities.
文摘The climate crisis necessitates the development of non-fossil energy sources.Harnessing solar energy for fuel production shows promise and offers the potential to utilize existing energy infrastructure.However,solar fuel production is in its early stages of development,constrained by low conversion efficiency and challenges in scaling up production.Concentrated solar energy(CSE)technology has matured alongside the rapid growth of solar thermal power plants.This review provides an overview of current CSE methods and solar fuel production,analyzes their integration compatibility,and delves into the theoretical mechanisms by which CSE impacts solar energy conversion efficiency and product selectivity in the context of photo-electrochemistry,thermochemistry,and photo-thermal co-catalysis for solar fuel production.The review also summarizes approaches to studying the photoelectric and photothermal effects of CSE.Lastly,it explores emerging novel CSE technology methods in the field of solar fuel production.
基金This work is financially supported by the National Natural Science Foundation of China (No. 20171036) and the Education Department of Shaanxi Province (No. 01JK229)
文摘The complex of samaric chloride lower hydrate with diethylammoniumdiethyldithiocarbamate (D-DDC) was synthesized conveniently in absolute alcohol and dry N_2atmosphere. The title complex was identified as Et_2NH_2[Sm(S_2CNEt_2)_4] by chemical and elementalanalyses, the bonding characteristics of which was characterized by IR. The enthalpies of solutionof samaric chloride hydrate and D-DDC in absolute alcohol at 298.15 K and the enthalpies change ofliquid-phase reaction of formation for Et_2NH_2[Sm(S_2CNEt_2)_4] at different temperatures weredetermined by mi-crocalorimetry. On the basis of experimental and calculated results, threethermodynamic parameters (the activation enthalpy, the activation entropy, and the activation freeenergy), the rate constant, and three kinetic parameters (the apparent activation energy, thepre-exponential constant, and the reaction order) of liquid phase reaction of formation wereobtained. The enthalpy change of the solid-phase title reaction at 298.15 K was calculated by athermochemical cycle.
文摘The complex of neodymium chloride lower hydrate with diethylammonium diethyldithiocarbamate (D-DDC) was synthesized conveniently in absolute alcohol and dry N_2 atmosphere. The title complex was identified as Et_2NH_2[Nd(S_2CNEt_2)_4] by chemical and elemental analyses and the bonding characteristics of which was characterized by IR. The enthalpies of solution of neodymium chloride hydrate and D-DDC in absolute alcohol at 298.15 K and the enthalpies change of liquid-phase reaction of formation for Et_2NH_2[Nd (S_2CNEt_2)_4] at different temperatures were determined by microcalorimetry. On the basis of experimental and calculated results, three thermodynamic parameters (the activation enthalpy, the activation entropy and the activation free energy), the rate constant and three kinetic parameters (the apparent activation energy, the pre-exponential constant and the reaction order) of liquid-phase reaction of formation were obtained. The enthalpy change of the solid-phase title reaction at 298.15 K was calculated by a thermochemical cycle.
基金National Natural Science Foundation of China(51905536)Natural Science Foundation of Tianjin(22JCYBJC01280)Key Project of Natural Science of Fundamental Research Funds for the Central Universities of China(3122023039).
文摘This paper investigated on influence of different alloying elements added into duplex stainless steel (DSS) on phase transitions using thermochemical methods in comparison with experiment.The results showed that the most possible species in the ferrite phase,austenite phase,σphase,Hcp phase,χphase,and carbide were Cr:Va-type,Fe:Va-type,Ni:Cr:Mo-type,Cr_(2)N-type,Fe_(24)Mo_(10)Cr_(24)-type,and Cr:Mo:C-type,respectively.Furthermore,the Ni,N,Cr,and Mo alloying had significant influences on the transition of each DSS phase.The Ni and N additions obviously raised the temperature at ferrite-1/austenite-1 balance while the Cr and Mo decreased the dual-phase balance temperature.In addition,the Ni addition can promote the precipitating ofσphase at relatively high temperature while the precipitating of Hcp phase at relatively low temperature.The Hcp phase andχphase can be obviously increased by the N addition.The introduction of Cr and Mo notably enhances the precipitation ofσphase.However,the promotion ofχphase precipitation is facilitated by the presence of Mo,while the Cr element acts as an inhibitor forχphase precipitation.Furthermore,the ferrite/austenite ratio tested by experiment was higher than that calculated by thermochemical methods,thus pre-designed solution temperature should be lower about 30-100℃than that calculated by thermochemical methods.
