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| 1 | Isotype Heterojunction‑Boosted CO_(2) Photoreduction to CO显示文摘Photocatalytic conversion of CO_(2) to high-value products plays a crucial role in the global pursuit of carbon–neutral economy.Junction photocatalysts,such as the isotype heterojunctions,offer an ideal paradigm to navigate the photocatalytic CO_(2) reduction reaction(CRR).Herein,we elucidate the behaviors of isotype heterojunctions toward photocatalytic CRR over a representative photocatalyst,g-C_(3)N_(4).Impressively,the isotype heterojunctions possess a significantly higher efficiency for the spatial separation and transfer of photogenerated carriers than the single components.Along with the intrinsically outstanding stability,the isotype heterojunctions exhibit an exceptional and stable activity toward the CO_(2) photoreduction to CO.More importantly,by combining quantitative in situ technique with the first-principles modeling,we elucidate that the enhanced photoinduced charge dynamics promotes the production of key intermediates and thus the whole reaction kinetics. | Chaogang Ban Youyu Duan Yang Wang Jiangping Ma Kaiwen Wang Jiazhi Meng Xue Liu Cong Wang Xiaodong Han Guozhong Cao Liyong Gan Xiaoyuan Zhou | 2022 | Nano-Micro Letters2022，14，5： | 2 |
| 2 | Bismuth clusters pinned on TiO_(2) porous nanowires boosting charge transfer for CO_(2) photoreduction to CH_(4)显示文摘Artificial photosynthesis in carbon dioxide(CO_(2))conversion into value-added chemicals attracts considerable attention but suffers from the low activity induced by sluggish separation of photogenerated carriers and the kinetic bottleneck-induced unsatisfied selectivity.Herein,we prepare a new-style Bi/TiO_(2) catalyst formed by pinning bismuth clusters on TiO_(2) nanowires through being confined by pores,which exhibits high activity and selectivity towards photocatalytic production of CH_(4) from CO_(2).Boosted charge transfer from TiO_(2) through Bi to the reactants is revealed via in situ X-ray photon spectroscopy and time-resolved photoluminescence(PL).Further,in situ Fourier transform infrared results confirm that Bi/TiO_(2) not only overcomes the multi-electron kinetics challenge of CO_(2) to CH_(4) via boosting charge transfer,but also facilitates proton production and transfer as well as the intermediates*CHO and*CH_(3)O generation,ultimately achieving the tandem catalysis towards methanation.Theoretical calculation also underlies that the more favorable reaction step from*CO to*CHO on Bi/TiO_(2) results in CH_(4) production with higher selectivity.Our work brings new insights into rational design of photocatalysts with high performance and the formation mechanism of CO_(2) to CH_(4) for solar energy storage in future. | Jiazhi Meng Kaiwen Wang Yang Wang Jiangping Ma Chaogang Ban Yajie Feng Bin Zhang Kai Zhou Liyong Gan Guang Han Danmei Yu Xiaoyuan Zhou | 2024 | Nano Research2024，17，3： | 0 |
| 3 | Strongly Coupled Ag/Sn-SnO_(2)Nanosheets Toward CO_(2)Electroreduction to Pure HCOOH Solutions at Ampere‑Level Current显示文摘Electrocatalytic reduction of CO_(2) converts intermittent renewable electricity into value-added liquid products with an enticing prospect,but its practical application is hampered due to the lack of high-performance electrocatalysts.Herein,we elaborately design and develop strongly coupled nanosheets composed of Ag nanoparticles and Sn-SnO_(2) grains,designated as Ag/Sn-SnO_(2) nanosheets(NSs),which possess optimized electronic structure,high electrical conductivity,and more accessible sites.As a result,such a catalyst exhibits unprecedented catalytic performance toward CO_(2)-to-formate conversion with near-unity faradaic efficiency(≥90%),ultrahigh partial current density(2,000 mA cm^(−2)),and superior long-term stability(200 mA cm^(−2),200 h),surpassing the reported catalysts of CO_(2) electroreduction to formate.Additionally,in situ attenuated total reflection-infrared spectra combined with theoretical calculations revealed that electron-enriched Sn sites on Ag/Sn-SnO_(2)NSs not only promote the formation of*OCHO and alleviate the energy barriers of*OCHO to*HCOOH,but also impede the desorption of H*.Notably,the Ag/Sn-SnO_(2)NSs as the cathode in a membrane electrode assembly with porous solid electrolyte layer reactor can continuously produce~0.12 M pure HCOOH solution at 100 mA cm^(−2)over 200 h.This work may inspire further development of advanced electrocatalysts and innovative device systems for promoting practical application of producing liquid fuels from CO_(2). | Min Zhang Aihui Cao Yucui Xiang Chaogang Ban Guang Han Junjie Ding Li‑Yong Gan Xiaoyuan Zhou | 2024 | Nano-Micro Letters2024，16，3： | 0 |
| 4 | A new insight into the promoting effects of transition metal phosphides in methanol electrooxidation显示文摘The construction of highly active catalysts for methanol oxidation reaction(MOR)is central to direct methanol fuel cells.Tremendous progress has been made in transition metal phosphides(TMPs)based catalysts.However,TMPs would be partially damaged and transformed into new substances(e.g.,Pt-M-P composite,where M represents a second transition metal)during Pt deposition process.This would pose a large obstacle to the cognition of the real promoting effects of TMPs in MOR.Herein,Co_(2)P co-catalysts(Pt-P/Co_(2)P@NPC,where NPC stands for N and P co-doped carbon)and Pt-Co-P composite catalysts(Pt-CoP/NPC)were controllably synthesized.Electrocatalysis tests show that the Pt-Co-P/NPC exhibits superior MOR activity as high as 1016 m A/mg_(Pt),significantly exceeding that of Pt-P/Co_(2)P@NPC(345 m A/mg_(Pt)).This result indicates that the promoting effect is ascribed primarily to the resultant Pt-Co-P composite,in sharply contrast to previous viewpoint that Co_(2)P itself improves the activity.Further mechanistic studies reveal that Pt-Co-P/NPC exhibits much stronger electron interaction and thus manifesting a remarkably weaker CO absorption than Pt-P/Co_(2)P@NPC and Pt/C.Moreover,Pt-Co-P is also more capable of producing oxygen-containing adsorbate and thus accelerating the removal of surface-bonded CO^(*),ultimately boosting the MOR performance. | Junjie Ding Shaojie Jing Changqing Yin Chaogang Ban Kaiwen Wang Xue Liu Youyu Duan Yuxin Zhang Guang Han Liyong Gan Jinsong Rao | 2023 | Chinese Chemical Letters2023，34，6： | 0 |
| 5 | Regulating local coordination environment of Mg-Co single atom catalyst for improved direct methanol fuel cell cathode显示文摘Fuel cells operated with a reformate fuel such as methanol are promising power systems for portable electronic devices due to their high safety,high energy density and low pollutant emissions.However,several critical issues including methanol crossover effect,CO-tolerance electrode and efficient oxygen reduction electrocatalyst with low or non-platinum usage have to be addressed before the direct methanol fuel cells(DMFCs)become commercially available for industrial application.Here,we report a highly active and selective Mg-Co dualsite oxygen reduction reaction(ORR)single atom catalyst(SAC)with porous N-doped carbon as the substrate.The catalyst exhibits a commercial Pt/C-comparable half-wave potential of 0.806 V(versus the reversible hydrogen electrode)in acid media with good stability.Furthermore,practical DMFCs test achieves a peak power density of over 200 m W cm^(-2)that far exceeds that of commercial Pt/C counterpart(82 m W cm^(-2)).Particularly,the Mg-Co DMFC system runs over 10 h with negligible current loss under 10 M concentration methanol work condition.Experimental results and theoretical calculations reveal that the N atom coordinated by Mg and Co atom exhibits an unconventional d-band-ditto localized p-band and can promote the dissociation of the key intermediate*OOH into*O and*OH,which accounts for the near unity selective 4e-ORR reaction pathway and enhanced ORR activity.In contrast,the N atom in SAC–Co remains inert in the absorption and desorption of*OOH and*OH.This local coordination environment regulation strategy around active sites may promote rational design of high-performance and durable fuel cell cathode electrocatalysts. | Kaiwen Wang Hanjun Zou Jiazhi Meng Chaogang Ban Xue Liu Jiangping Ma Cong Wang Liyong Gan Xiaodong Han Xiaoyuan Zhou | 2023 | Journal of Magnesium and Alloys2023，11，6： | 0 |
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