Catalyst-aided regeneration is a promising method for reducing the high regeneration energy consumption of amine-based CO_(2)capture technologies.However,the intrinsic relationship between the properties of the acidic...Catalyst-aided regeneration is a promising method for reducing the high regeneration energy consumption of amine-based CO_(2)capture technologies.However,the intrinsic relationship between the properties of the acidic sites and their catalytic activity is controversial.In this study,a series of W-based catalysts supported by ZrTiO_(x)were synthesised,and the effects of the intensity,distribution,and type of acid sites were systematically investigated by quantitatively regulating the acidic site properties.The results indicate stronger acidic sites play a more important role in the catalytic reaction.Moreover,the catalysts showed excellent performance only if the Br?nsted acid sites(BASs)and Lewis acid sites(LASs)coexisted.During the catalytic reaction,the BASs facilitated deprotonation,and the LASs promoted the decomposition of carbamates.The ratio of BASs to LASs(B/L)was a critical factor for catalytic activity,wherein optimal performance was achieved when the B/L ratio was close to 1.The 10%HPW/ZrTiO_(x)composite performed better than WO_(3)/ZrTiO_(x)and HSiW/ZrTiO_(x)because it had a stronger acid intensity and a suitable B/L ratio.As a result,the relative heat duty was reduced by 47%compared to 30%aqueous MEA,and the maximum CO_(2)desorption rate was increased by 83%.The Bader charge indicated that the W atoms of HPW/ZrTiO_(x)lost more electrons(0.18)than those of WO_(3)/ZrTiO_(x),which can weaken the O±H bond energy.Consequently,the calculated deprotonation energy is as low as 257 kJ mol^(-1)for HPW/ZrTiO_(x).展开更多
Catalytic regeneration is a key approach to solving high energy consumption issues in the amine-based CO_(2)absorption method.Previous studies have shown that loaded acid sites(such as SO_(4)^(2-))are beneficial for p...Catalytic regeneration is a key approach to solving high energy consumption issues in the amine-based CO_(2)absorption method.Previous studies have shown that loaded acid sites(such as SO_(4)^(2-))are beneficial for promoting low-temperature CO_(2)-rich amine regeneration,but their weak binding strength to the support results in limited catalyst life.Herein,we proposed an advanced catalyst modification strategy to maintain the active hydroxyl group(Zr-OH-Fe)via actively transferring electrons on the surface of FeZrO_(x)nano-heterojunction.Combining in situ DRIFTS and DFT calculations,we revealed that the ZrOH-Fe at the ZrO_(2)-Fe_(2)O_(3)heterointerfaces exhibit enhanced proton-donating ability,with deprotonation energy reduced from 2.94 to 2.61 eV compared to Zr-OH(which should be called inert hydroxyl group).This improvement favors the rate-determining proton transfer step from RNH_(3)^(+)to RNHCOO^(-).Surprisingly,it increased the CO_(2)desorption rate by 10.5 times and reduced the energy consumption by 43.6%during amine regeneration.This work offers a practical strategy for improving the performance of lowtemperature CO_(2)-rich amine regeneration catalysts,and the low-cost recyclability of amine used in CO_(2)capture.展开更多
Runx2 is a major regulator of osteoblast differentiation and function;however,the role of Runx2 in peripheral nerve repair is unclea r.Here,we analyzed Runx2expression following injury and found that it was specifical...Runx2 is a major regulator of osteoblast differentiation and function;however,the role of Runx2 in peripheral nerve repair is unclea r.Here,we analyzed Runx2expression following injury and found that it was specifically up-regulated in Schwann cells.Furthermore,using Schwann cell-specific Runx2 knocko ut mice,we studied peripheral nerve development and regeneration and found that multiple steps in the regeneration process following sciatic nerve injury were Runx2-dependent.Changes observed in Runx2 knoc kout mice include increased prolife ration of Schwann cells,impaired Schwann cell migration and axonal regrowth,reduced re-myelination of axo ns,and a block in macrophage clearance in the late stage of regeneration.Taken together,our findings indicate that Runx2 is a key regulator of Schwann cell plasticity,and therefore peripheral nerve repair.Thus,our study shows that Runx2 plays a major role in Schwann cell migration,re-myelination,and peripheral nerve functional recovery following injury.展开更多
CO_(2)-to-formate electrosynthesis with high selectivity and stability has been a long-sought objective.Unfortunately,most catalysts undergo structural and valence state changes due to surface oxidation during operati...CO_(2)-to-formate electrosynthesis with high selectivity and stability has been a long-sought objective.Unfortunately,most catalysts undergo structural and valence state changes due to surface oxidation during operation or storage,resulting in decreased catalytic performance.Herein,we report a efficient and stable BiIn@Cu-foam electrode through the in-situ regeneration of Bi^(0) active sites to renew the surface activation.The electronic structure of Bi site can be regulated by introducing In,thereby enhancing the adsorption strength of*OCHO.The optimized electrode exhibits over 90%FE_(formate)at a wide potential window(-0.9–-2.2 V),and formation rate for 3.15 mM cm^(-1)h^(-1).Especially,the electrode can maintain the high performance at continuously electrolysis for more than 300 h,or for more than 50 cycles,even repeated operation and storage for more than 2 years.This work provides a promising candidate and new insight to construct industrially viable stable Bi-based catalyst for formate electrosynthesis.展开更多
基金supported by the National Natural Science Foundation of China(No.52100133,No.52222005)the Key R&D Program of Yunnan Province(No.202303AC100008)。
文摘Catalyst-aided regeneration is a promising method for reducing the high regeneration energy consumption of amine-based CO_(2)capture technologies.However,the intrinsic relationship between the properties of the acidic sites and their catalytic activity is controversial.In this study,a series of W-based catalysts supported by ZrTiO_(x)were synthesised,and the effects of the intensity,distribution,and type of acid sites were systematically investigated by quantitatively regulating the acidic site properties.The results indicate stronger acidic sites play a more important role in the catalytic reaction.Moreover,the catalysts showed excellent performance only if the Br?nsted acid sites(BASs)and Lewis acid sites(LASs)coexisted.During the catalytic reaction,the BASs facilitated deprotonation,and the LASs promoted the decomposition of carbamates.The ratio of BASs to LASs(B/L)was a critical factor for catalytic activity,wherein optimal performance was achieved when the B/L ratio was close to 1.The 10%HPW/ZrTiO_(x)composite performed better than WO_(3)/ZrTiO_(x)and HSiW/ZrTiO_(x)because it had a stronger acid intensity and a suitable B/L ratio.As a result,the relative heat duty was reduced by 47%compared to 30%aqueous MEA,and the maximum CO_(2)desorption rate was increased by 83%.The Bader charge indicated that the W atoms of HPW/ZrTiO_(x)lost more electrons(0.18)than those of WO_(3)/ZrTiO_(x),which can weaken the O±H bond energy.Consequently,the calculated deprotonation energy is as low as 257 kJ mol^(-1)for HPW/ZrTiO_(x).
基金financially supported by the National Natural Science Foundation of China(52222005,52100133)the Key R&D Program of Yunnan Province(202303AC100008)。
文摘Catalytic regeneration is a key approach to solving high energy consumption issues in the amine-based CO_(2)absorption method.Previous studies have shown that loaded acid sites(such as SO_(4)^(2-))are beneficial for promoting low-temperature CO_(2)-rich amine regeneration,but their weak binding strength to the support results in limited catalyst life.Herein,we proposed an advanced catalyst modification strategy to maintain the active hydroxyl group(Zr-OH-Fe)via actively transferring electrons on the surface of FeZrO_(x)nano-heterojunction.Combining in situ DRIFTS and DFT calculations,we revealed that the ZrOH-Fe at the ZrO_(2)-Fe_(2)O_(3)heterointerfaces exhibit enhanced proton-donating ability,with deprotonation energy reduced from 2.94 to 2.61 eV compared to Zr-OH(which should be called inert hydroxyl group).This improvement favors the rate-determining proton transfer step from RNH_(3)^(+)to RNHCOO^(-).Surprisingly,it increased the CO_(2)desorption rate by 10.5 times and reduced the energy consumption by 43.6%during amine regeneration.This work offers a practical strategy for improving the performance of lowtemperature CO_(2)-rich amine regeneration catalysts,and the low-cost recyclability of amine used in CO_(2)capture.
基金supported by the National Natural Science Foundation of China,No.82104795 (to RH)。
文摘Runx2 is a major regulator of osteoblast differentiation and function;however,the role of Runx2 in peripheral nerve repair is unclea r.Here,we analyzed Runx2expression following injury and found that it was specifically up-regulated in Schwann cells.Furthermore,using Schwann cell-specific Runx2 knocko ut mice,we studied peripheral nerve development and regeneration and found that multiple steps in the regeneration process following sciatic nerve injury were Runx2-dependent.Changes observed in Runx2 knoc kout mice include increased prolife ration of Schwann cells,impaired Schwann cell migration and axonal regrowth,reduced re-myelination of axo ns,and a block in macrophage clearance in the late stage of regeneration.Taken together,our findings indicate that Runx2 is a key regulator of Schwann cell plasticity,and therefore peripheral nerve repair.Thus,our study shows that Runx2 plays a major role in Schwann cell migration,re-myelination,and peripheral nerve functional recovery following injury.
基金supported by the National Natural Science Foundation of China(22238013 and 22178393)Postdoctoral Science Foundation of Central South University(320808)+1 种基金Natural Science Foundation of Hunan Province(2023JJ40706)the High Performance Computing Center of Central South University。
文摘CO_(2)-to-formate electrosynthesis with high selectivity and stability has been a long-sought objective.Unfortunately,most catalysts undergo structural and valence state changes due to surface oxidation during operation or storage,resulting in decreased catalytic performance.Herein,we report a efficient and stable BiIn@Cu-foam electrode through the in-situ regeneration of Bi^(0) active sites to renew the surface activation.The electronic structure of Bi site can be regulated by introducing In,thereby enhancing the adsorption strength of*OCHO.The optimized electrode exhibits over 90%FE_(formate)at a wide potential window(-0.9–-2.2 V),and formation rate for 3.15 mM cm^(-1)h^(-1).Especially,the electrode can maintain the high performance at continuously electrolysis for more than 300 h,or for more than 50 cycles,even repeated operation and storage for more than 2 years.This work provides a promising candidate and new insight to construct industrially viable stable Bi-based catalyst for formate electrosynthesis.
