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
Apoptosis preserves organismal homeostasis by selectively eliminating unnecessary or damaged cells, with accumulating evidence also suggesting that it activates regenerative pathways and facilitates tissue remodeling....Apoptosis preserves organismal homeostasis by selectively eliminating unnecessary or damaged cells, with accumulating evidence also suggesting that it activates regenerative pathways and facilitates tissue remodeling. To date, however, the regulatory mechanisms linking this form of programmed cell death to regeneration remain poorly defined, particularly in evolutionarily basal organisms. Using the sea cucumber (Apostichopus japonicus) as a model for intestinal regeneration, this study identified robust apoptotic activity across key regenerative stages. Pharmacological suppression of apoptosis during wound healing and mesenteric scaffold formation critically impaired intestinal regeneration. Quantitative proteomics using direct data-independent acquisition (DIA) revealed coordinated down-regulation of lipid metabolic pathways under apoptosis-inhibited conditions, with notable suppression of Ca^(2+)-independent phospholipase A2 (iPLA2), an enzyme typically up-regulated during successful regeneration. In parallel, expression of regeneration-associated factors WNT6 and EGFL7 was markedly reduced under apoptotic blockade. Targeted inhibition of iPLA2, EGFL7, or WNT6 each resulted in impaired mesenteric outgrowth and reduced proliferative activity within the regenerating intestinal primordia. Collectively, these findings suggest two potential mechanistic pathways: apoptosis-mediated regeneration of lipid metabolism via iPLA2 and apoptosis-dependent activation of WNT6/EGFL7 signaling. This study provides mechanistic insight into apoptosis-coupled regenerative processes in basal deuterostomes and expands the conceptual framework of programmed cell death in tissue renewal.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
为探究稻茬小麦深施肥“一基一追”机艺融合技术的增产增效减排机制,2021—2024年在长江下游南通稻茬麦区开展大田试验。试验采用缓释掺混肥料(SRF,N∶P_(2)O_(5)∶K_(2)O=26∶12∶12)和普通尿素(U,46%N),结合自主研发的2BFGK-12(6)260...为探究稻茬小麦深施肥“一基一追”机艺融合技术的增产增效减排机制,2021—2024年在长江下游南通稻茬麦区开展大田试验。试验采用缓释掺混肥料(SRF,N∶P_(2)O_(5)∶K_(2)O=26∶12∶12)和普通尿素(U,46%N),结合自主研发的2BFGK-12(6)260全秸秆茬地洁区旋耕智能施肥播种机和3ZF-4(200)中耕追肥机,设置7种施肥模式(30 cm+15 cm宽窄行种植):以尿素4次分施(N 240 kg hm^(-2),基肥∶分蘖肥∶拔节肥∶孕穗肥=5∶1∶2∶2,窄行基施,追肥全田撒施)为对照(CK);减氮15%(N 204 kg hm^(-2))条件下设置6种处理:M_(1)(100%SRF窄行基施);M_(2)(60%SRF窄行基施+40%U拔节期窄行撒施);M_(3)(60%SRF窄行基施+40%U返青期宽行条施);M_(4)(60%SRF窄行基施+40%SRF返青期窄行撒施);M_(5)(60%SRF窄行基施+40%SRF返青期宽行条施);M_(4+5)(60%SRF窄行基施+20%SRF返青期宽行条施+20%SRF返青期窄行撒施)。研究比较不同施肥模式对小麦产量效益、根系形态生理、氮素利用效率及N_(2)O排放的影响。结果表明,与CK相比,M_(2)~M_(5)处理提高了小麦产量(4.0%~19.0%)和经济效益(13.7%~35.7%),其中M_(4)和M_(5)处理表现最优,分别增产14.1%和19.0%,经济效益提升34.5%和35.7%。这些处理明显改善了根系特性(根干重密度增加9.7%~111.8%,根系活力和氧化力分别提高6.8%~52.0%和4.2%~44.2%),降低N_(2)O累积排放量22.6%~34.5%,提高0~20 cm土层硝态氮含量11.2%~40.0%。在氮素利用方面,M_(2)~M_(5)处理均提高了籽粒氮素积累量、花后氮素积累量及其对籽粒氮素的贡献率,氮肥利用效率指标(包括偏生产力、农学效率和表观利用率)分别显著提升了22.4%~40.0%、29.7%~74.3%和9.41~18.77个百分点。值得注意的是,M_(4)和M_(5)处理表现出最优的综合效益:N_(2)O累积排放量降幅最大(分别达27.0%和34.5%),氮肥表观利用率2季均维持在43.0%以上(均值分别为43.5%和46.8%),同时在生育后期保持较高的根系活性和耕层无机氮含量。相比之下,M_(1)处理虽然实现了最大的N_(2)O减排效果(降幅35.9%),但导致减产10.4%和经济效益下降10.8%,且氮肥利用效率呈现不稳定的年际变化特征。而优化处理M_(4+5)进一步改善了根系形态生理特性,并提高氮肥表观利用率和籽粒氮素积累量。综上,减氮15%条件下(N 204 kg hm^(-2)),缓混肥2次施用处理(M_(4)和M_(5))能实现产量、经济效益、氮肥利用效率和N_(2)O减排的协同提高,并以追肥深施处理(M_(5))效应更强。本研究为稻茬小麦缓释肥减氮优化高效应用提供重要理论依据。展开更多
P2型层状过渡金属氧化物(P2-Na_(x)TMO_(2))因其优异的循环稳定性和倍率性能,成为钠离子电池正极材料的有力候选者。然而,其在高电压下的不可逆相变和固有低理论容量问题,阻碍了实际应用。本研究工作提出高熵策略与双相结构的协同设计...P2型层状过渡金属氧化物(P2-Na_(x)TMO_(2))因其优异的循环稳定性和倍率性能,成为钠离子电池正极材料的有力候选者。然而,其在高电压下的不可逆相变和固有低理论容量问题,阻碍了实际应用。本研究工作提出高熵策略与双相结构的协同设计来克服这些挑战。通过在P2相高熵基体中引入O3相,构建新型P2/O3双相高熵层状氧化物Na_(0.70)Ni_(0.25)Mn_(0.35)Co_(0.15)Fe_(0.05)Ti_(0.20)O_(2)(简称Na_(0.70)NMCFT)。其中,高熵设计通过构型熵稳定效应有效抑制P2相的不可逆相变,而O3相则通过协同作用弥补容量不足并提升循环稳定性。此外,双相组分之间的相互作用进一步促进P2-O3与P2-P3相变的高度可逆性。Na_(0.70)NMCFT在1C倍率下的初始放电容量为102.08 mAhg^(-1),200次循环后容量保持率达88.15%,表明具有优异的循环稳定性。更重要的是,即使在10C的高倍率下,Na_(0.70)NMCFT仍能提供85.67 mAh g^(-1)的初始放电比容量,并在1000次循环后容量保持率达70%。本工作证实双相高熵设计在提升钠离子电池正极性能中的关键作用,为开发先进钠离子电池正极材料提供了新思路。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supported by the National Natural Science Foundation of China(32325050)Natural Science Foundation of Zhejiang Province(LQN25C190013)+2 种基金State Key Program of Natural Science Foundation of Ningbo(2023J005)General Projects of Zhejiang Provincial Department of Education(Y202456633)K.C.Wong Magna Fund in Ningbo University。
文摘Apoptosis preserves organismal homeostasis by selectively eliminating unnecessary or damaged cells, with accumulating evidence also suggesting that it activates regenerative pathways and facilitates tissue remodeling. To date, however, the regulatory mechanisms linking this form of programmed cell death to regeneration remain poorly defined, particularly in evolutionarily basal organisms. Using the sea cucumber (Apostichopus japonicus) as a model for intestinal regeneration, this study identified robust apoptotic activity across key regenerative stages. Pharmacological suppression of apoptosis during wound healing and mesenteric scaffold formation critically impaired intestinal regeneration. Quantitative proteomics using direct data-independent acquisition (DIA) revealed coordinated down-regulation of lipid metabolic pathways under apoptosis-inhibited conditions, with notable suppression of Ca^(2+)-independent phospholipase A2 (iPLA2), an enzyme typically up-regulated during successful regeneration. In parallel, expression of regeneration-associated factors WNT6 and EGFL7 was markedly reduced under apoptotic blockade. Targeted inhibition of iPLA2, EGFL7, or WNT6 each resulted in impaired mesenteric outgrowth and reduced proliferative activity within the regenerating intestinal primordia. Collectively, these findings suggest two potential mechanistic pathways: apoptosis-mediated regeneration of lipid metabolism via iPLA2 and apoptosis-dependent activation of WNT6/EGFL7 signaling. This study provides mechanistic insight into apoptosis-coupled regenerative processes in basal deuterostomes and expands the conceptual framework of programmed cell death in tissue renewal.
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.
文摘为探究稻茬小麦深施肥“一基一追”机艺融合技术的增产增效减排机制,2021—2024年在长江下游南通稻茬麦区开展大田试验。试验采用缓释掺混肥料(SRF,N∶P_(2)O_(5)∶K_(2)O=26∶12∶12)和普通尿素(U,46%N),结合自主研发的2BFGK-12(6)260全秸秆茬地洁区旋耕智能施肥播种机和3ZF-4(200)中耕追肥机,设置7种施肥模式(30 cm+15 cm宽窄行种植):以尿素4次分施(N 240 kg hm^(-2),基肥∶分蘖肥∶拔节肥∶孕穗肥=5∶1∶2∶2,窄行基施,追肥全田撒施)为对照(CK);减氮15%(N 204 kg hm^(-2))条件下设置6种处理:M_(1)(100%SRF窄行基施);M_(2)(60%SRF窄行基施+40%U拔节期窄行撒施);M_(3)(60%SRF窄行基施+40%U返青期宽行条施);M_(4)(60%SRF窄行基施+40%SRF返青期窄行撒施);M_(5)(60%SRF窄行基施+40%SRF返青期宽行条施);M_(4+5)(60%SRF窄行基施+20%SRF返青期宽行条施+20%SRF返青期窄行撒施)。研究比较不同施肥模式对小麦产量效益、根系形态生理、氮素利用效率及N_(2)O排放的影响。结果表明,与CK相比,M_(2)~M_(5)处理提高了小麦产量(4.0%~19.0%)和经济效益(13.7%~35.7%),其中M_(4)和M_(5)处理表现最优,分别增产14.1%和19.0%,经济效益提升34.5%和35.7%。这些处理明显改善了根系特性(根干重密度增加9.7%~111.8%,根系活力和氧化力分别提高6.8%~52.0%和4.2%~44.2%),降低N_(2)O累积排放量22.6%~34.5%,提高0~20 cm土层硝态氮含量11.2%~40.0%。在氮素利用方面,M_(2)~M_(5)处理均提高了籽粒氮素积累量、花后氮素积累量及其对籽粒氮素的贡献率,氮肥利用效率指标(包括偏生产力、农学效率和表观利用率)分别显著提升了22.4%~40.0%、29.7%~74.3%和9.41~18.77个百分点。值得注意的是,M_(4)和M_(5)处理表现出最优的综合效益:N_(2)O累积排放量降幅最大(分别达27.0%和34.5%),氮肥表观利用率2季均维持在43.0%以上(均值分别为43.5%和46.8%),同时在生育后期保持较高的根系活性和耕层无机氮含量。相比之下,M_(1)处理虽然实现了最大的N_(2)O减排效果(降幅35.9%),但导致减产10.4%和经济效益下降10.8%,且氮肥利用效率呈现不稳定的年际变化特征。而优化处理M_(4+5)进一步改善了根系形态生理特性,并提高氮肥表观利用率和籽粒氮素积累量。综上,减氮15%条件下(N 204 kg hm^(-2)),缓混肥2次施用处理(M_(4)和M_(5))能实现产量、经济效益、氮肥利用效率和N_(2)O减排的协同提高,并以追肥深施处理(M_(5))效应更强。本研究为稻茬小麦缓释肥减氮优化高效应用提供重要理论依据。
文摘P2型层状过渡金属氧化物(P2-Na_(x)TMO_(2))因其优异的循环稳定性和倍率性能,成为钠离子电池正极材料的有力候选者。然而,其在高电压下的不可逆相变和固有低理论容量问题,阻碍了实际应用。本研究工作提出高熵策略与双相结构的协同设计来克服这些挑战。通过在P2相高熵基体中引入O3相,构建新型P2/O3双相高熵层状氧化物Na_(0.70)Ni_(0.25)Mn_(0.35)Co_(0.15)Fe_(0.05)Ti_(0.20)O_(2)(简称Na_(0.70)NMCFT)。其中,高熵设计通过构型熵稳定效应有效抑制P2相的不可逆相变,而O3相则通过协同作用弥补容量不足并提升循环稳定性。此外,双相组分之间的相互作用进一步促进P2-O3与P2-P3相变的高度可逆性。Na_(0.70)NMCFT在1C倍率下的初始放电容量为102.08 mAhg^(-1),200次循环后容量保持率达88.15%,表明具有优异的循环稳定性。更重要的是,即使在10C的高倍率下,Na_(0.70)NMCFT仍能提供85.67 mAh g^(-1)的初始放电比容量,并在1000次循环后容量保持率达70%。本工作证实双相高熵设计在提升钠离子电池正极性能中的关键作用,为开发先进钠离子电池正极材料提供了新思路。
