This future article discusses the new prospects and directions of CO_(2)conversion via the photo-electrocatalytic(PEC)route.The second(2nd)generation solar fuels and chemicals(SFs)are generated directly in PEC systems...This future article discusses the new prospects and directions of CO_(2)conversion via the photo-electrocatalytic(PEC)route.The second(2nd)generation solar fuels and chemicals(SFs)are generated directly in PEC systems via electrons/protons reactions without forming molecular H_(2)as an intermediate,overcoming the thermodynamics limitations and practical issues encountered for electro-fuels produced by multistep thermocatalytic processes(i.e.CO_(2)conversion with H_(2)coming from water electrolysis).A distributed and decentralized production of SFs requires very compact,highly integrated,and intensified technologies.Among the existing reactors of advanced design(based on artificial leaves or photosynthesis),the integrated photovoltaic plus electrocatalytic(PV-EC)device is the only system(demonstrated at large scale)to produce SFs with high solar-to-fuel(STF)efficiency.However,while the literature indicates STF efficiency as the main(and only)measure of process performance,we remark here the need to refer to productivity(in terms of current density)and make tests with reliable flow PEC systems(with electrodes of at least 5–10 cm^(2))to accelerate the scaling-up process.Using approaches that minimize downstream separation costs is also mandatory.Many limitations exist in PEC systems,but most can be overcome by proper electrode and cell engineering,thus going beyond the properties of the electrocatalysts.As examples of current developments,we present the progress of(i)artificial leaf/tree devices for green H_(2)distributed production and(ii)a PEC device producing the same chemicals at both cathode and anode parts without downstream operations for green solvent distributed production.Based on these developments,future directions,such as producing fertilizers and food components from the air,are outlined.The aim is to provide new ideas and research directions from a personal perspective.展开更多
为了理解甲醇/柴油双燃料机的自燃特性并为燃烧计算所需骨架机理提供理论依据,以正庚烷作为柴油替代物,应用快速压缩机对宽广实验条件下甲醇/正庚烷混合燃料的自燃特性进行了研究。实验条件覆盖了甲醇/柴油双燃料机的典型工况。实验研...为了理解甲醇/柴油双燃料机的自燃特性并为燃烧计算所需骨架机理提供理论依据,以正庚烷作为柴油替代物,应用快速压缩机对宽广实验条件下甲醇/正庚烷混合燃料的自燃特性进行了研究。实验条件覆盖了甲醇/柴油双燃料机的典型工况。实验研究结果显示,随着压力升高、甲醇比例减少或当量比增大,混合燃料滞燃期变短。根据实验数据验证了爱尔兰国立大学(National University of Ireland,NUI)的正庚烷详细机理对甲醇/正庚烷的适用性,并利用该机理在CHEMKIN PRO软件中进行了化学动力学分析。结果表明,甲醇与正庚烷竞争羟基(hydroxyl,OH)从而抑制系统氧化过程。敏感性分析结果显示,超氧化氢(HO_(2))反应生成过氧化氢(H_(2)O_(2))是燃烧过程中最敏感的反应,抑制系统氧化过程的进行。本研究可为获得适用于甲醇/柴油双燃料机燃烧计算的骨架机理提供理论依据。展开更多
Chemical non-equilibrium flow was investigated for the scramjet single expansion ramp nozzle(SERN)with a strut-based liquid-kerosene-fueled combustor.Two-dimensional Reynolds-averaged NavierStokes(RANS)equations were ...Chemical non-equilibrium flow was investigated for the scramjet single expansion ramp nozzle(SERN)with a strut-based liquid-kerosene-fueled combustor.Two-dimensional Reynolds-averaged NavierStokes(RANS)equations were solved with the species conservation equation for continuous phase and the renormalization group(RNG)k-εturbulence model.Lagrangian discrete-phase model was analyzed for liquidkerosene droplets behavior in the supersonic stream.Combustion was simulated by kerosene surrogate fuel's10-species and 13-step reduced reaction kinetics mechanism with use of Arrhenius's laminar finite rate model.Parametric studies were carried out to estimate the influence of different fuel injection positions and equivalent mixture ratios on the SERN chemical non-equilibrium effects.Numerical calculation results show that the strutbased combustor enables convenient modeling of various SERN entry conditions,which is similar with many preceding investigations,by changing the injector strut position and controlling the mass flow rate of each injector.Chemical non-equilibrium effects function in the whole SERN,especially in the initial flow expansion region,leads to obviously higher SERN performance of the non-equilibrium flow than that of the frozen flow.Furthermore,the distributed fuel injection pattern plays a significant role in enhancing the combustion efficiency in combustor,but weakening the chemical non-equilibrium effects funciton in SERN.Additionally,while the equivalent mixture ratio increases,the SERN thrust coefficient and lift coefficient rise gradually,and the increment of non-equilibrium flow in relation to frozen flow becomes higher as well.To be specific,the equivalent mixture ratio is 0.6,the maximum increment of thrust coefficient and lift coefficient are 11.6% and 25% respectively.展开更多
基金the EU for providing support to these activities through the EU projects DECADE(862030),EPOCH(101070976)and SCOPE(810182)。
文摘This future article discusses the new prospects and directions of CO_(2)conversion via the photo-electrocatalytic(PEC)route.The second(2nd)generation solar fuels and chemicals(SFs)are generated directly in PEC systems via electrons/protons reactions without forming molecular H_(2)as an intermediate,overcoming the thermodynamics limitations and practical issues encountered for electro-fuels produced by multistep thermocatalytic processes(i.e.CO_(2)conversion with H_(2)coming from water electrolysis).A distributed and decentralized production of SFs requires very compact,highly integrated,and intensified technologies.Among the existing reactors of advanced design(based on artificial leaves or photosynthesis),the integrated photovoltaic plus electrocatalytic(PV-EC)device is the only system(demonstrated at large scale)to produce SFs with high solar-to-fuel(STF)efficiency.However,while the literature indicates STF efficiency as the main(and only)measure of process performance,we remark here the need to refer to productivity(in terms of current density)and make tests with reliable flow PEC systems(with electrodes of at least 5–10 cm^(2))to accelerate the scaling-up process.Using approaches that minimize downstream separation costs is also mandatory.Many limitations exist in PEC systems,but most can be overcome by proper electrode and cell engineering,thus going beyond the properties of the electrocatalysts.As examples of current developments,we present the progress of(i)artificial leaf/tree devices for green H_(2)distributed production and(ii)a PEC device producing the same chemicals at both cathode and anode parts without downstream operations for green solvent distributed production.Based on these developments,future directions,such as producing fertilizers and food components from the air,are outlined.The aim is to provide new ideas and research directions from a personal perspective.
文摘为了理解甲醇/柴油双燃料机的自燃特性并为燃烧计算所需骨架机理提供理论依据,以正庚烷作为柴油替代物,应用快速压缩机对宽广实验条件下甲醇/正庚烷混合燃料的自燃特性进行了研究。实验条件覆盖了甲醇/柴油双燃料机的典型工况。实验研究结果显示,随着压力升高、甲醇比例减少或当量比增大,混合燃料滞燃期变短。根据实验数据验证了爱尔兰国立大学(National University of Ireland,NUI)的正庚烷详细机理对甲醇/正庚烷的适用性,并利用该机理在CHEMKIN PRO软件中进行了化学动力学分析。结果表明,甲醇与正庚烷竞争羟基(hydroxyl,OH)从而抑制系统氧化过程。敏感性分析结果显示,超氧化氢(HO_(2))反应生成过氧化氢(H_(2)O_(2))是燃烧过程中最敏感的反应,抑制系统氧化过程的进行。本研究可为获得适用于甲醇/柴油双燃料机燃烧计算的骨架机理提供理论依据。
文摘Chemical non-equilibrium flow was investigated for the scramjet single expansion ramp nozzle(SERN)with a strut-based liquid-kerosene-fueled combustor.Two-dimensional Reynolds-averaged NavierStokes(RANS)equations were solved with the species conservation equation for continuous phase and the renormalization group(RNG)k-εturbulence model.Lagrangian discrete-phase model was analyzed for liquidkerosene droplets behavior in the supersonic stream.Combustion was simulated by kerosene surrogate fuel's10-species and 13-step reduced reaction kinetics mechanism with use of Arrhenius's laminar finite rate model.Parametric studies were carried out to estimate the influence of different fuel injection positions and equivalent mixture ratios on the SERN chemical non-equilibrium effects.Numerical calculation results show that the strutbased combustor enables convenient modeling of various SERN entry conditions,which is similar with many preceding investigations,by changing the injector strut position and controlling the mass flow rate of each injector.Chemical non-equilibrium effects function in the whole SERN,especially in the initial flow expansion region,leads to obviously higher SERN performance of the non-equilibrium flow than that of the frozen flow.Furthermore,the distributed fuel injection pattern plays a significant role in enhancing the combustion efficiency in combustor,but weakening the chemical non-equilibrium effects funciton in SERN.Additionally,while the equivalent mixture ratio increases,the SERN thrust coefficient and lift coefficient rise gradually,and the increment of non-equilibrium flow in relation to frozen flow becomes higher as well.To be specific,the equivalent mixture ratio is 0.6,the maximum increment of thrust coefficient and lift coefficient are 11.6% and 25% respectively.