摘要：The design of non-noble metal heterogeneous catalyst with superior performance for selective hydrogenation or transfer hydrogenation of nitroarenes to amines is significant but ***,a single-atom Fe supported by nitrogen-doped carbon(Fe_(1)/N-C)catalyst is *** Fe_(1)/N-C sample shows superior performances for the selective hydrogenation and transfer hydrogenation of nitrobenzene to aniline at different *** functional theory(DFT)calculations show that the superior catalytic activity for the selective hydrogenation at lower temperatures could be attributed to the effective activation of the reactant and intermediates by the Fe_(1)/***,the excellent performance of Fe_(1)/N-C for the selective transfer hydrogenation could be attributed to that the reaction energy barrier for dehydrogenation of isopropanol can be overcome by elevated temperatures.

摘要：The development of low-cost semiconductor photocatalysts for highly efficient and durable photocatalytic H2 evolution under visible light is very *** this study,we combine low-cost metallic Ni3C cocatalysts with twin nanocrystal Zn0.5Cd0.5S(ZCS)solid solution homojunctions for an efficient visible-light-driven H2 production by a simple ***-synthesized Zn0.5Cd0.5S-1%Ni3C(ZCS-1)heterojunction/homojunction nanohybrid exhibited the highest photocatalytic H2-evolution rate of 783μmol h‒1 under visible light,which is 2.88 times higher than that of pristine twin nanocrystal ZCS solid *** apparent quantum efficiencies of ZCS and ZCS-1 are measured to be 6.13%and 19.25%at 420 nm,***,the homojunctions between the zinc blende and wurtzite segments in twin nanocrystal ZCS solid solution can significantly improve the light absorption and separation of photogenerated electron-hole ***,the heterojunction between ZCS and metallic Ni3C NP cocatalysts can efficiently trap excited electrons from ZCS solid solution and enhance the H2-evolution kinetics at the surface for improving catalytic *** study demonstrates a unique one-step strategy for constructing heterojunction/homojunction hybrid nanostructures for a more efficient photocatalytic H2 evolution compared to other noble metal photocatalytic systems.

摘要：Inspired by MXene nanosheets and their regulation of surface functional groups,a series of Ti_(2)C‐based single‐atom electrocatalysts(TM@Ti_(2)CT_(x),TM=V,Cr,Mn,Fe,Co,and Ni)with two dif‐ferent functional groups(T=–O and–S)was *** CO_(2)RR catalytic performance was stud‐ied using well‐defined ab initio *** results show that the CO_(2) molecule can be more readily activated on TM@Ti_(2)CO_(2) than the TM@Ti_(2)CS_(2) *** charge analysis reveals that the Ti_(2)CO_(2) substrate is involved in the adsorption reaction,and enough electrons are injected into the 2π*u orbital of CO_(2),leading to a V‐shaped CO_(2) molecular configuration and partial negative charge *** V‐shaped CO_(2) further reduces the difficulty of the first hydrogenation reac‐tion *** calculatedΔG of the first hydrogenation reaction on TM@Ti_(2)CO_(2) was significantly lower than that of the TM@Ti_(2)CS_(2) ***,the subsequent CO_(2) reduction pathways show that the UL of the potential determining step on TM@Ti_(2)CS_(2) is smaller than that of TM@Ti_(2)CO_(2).Combining the advantages of both TM@Ti_(2)CS_(2) and TM@Ti_(2)CO_(2),we designed a mixed functional group surface with–O and–S to anchor TM *** results show that Cr atoms an‐chored on the surface of mixed functional groups exhibit high catalytic activity for the selective production of *** study opens an exciting new avenue for the rational design of highly selec‐tive MXene‐based single‐atom CO_(2)RR electrocatalysts.

摘要：The hydrogenation of CO_(2) into methanol has attracted much attention and In_(2)O_(3) is a promising *** metal elements into In_(2)O_(3)(M/In_(2)O_(3))is one of the main strategies to improve its ***,its mechanism and active sites remain unclear and need to be further ***,the noble‐metal‐free In_(x)‐Co_(y) oxides catalysts were ***‐improved performance and obvious product selectivity shift were *** optimized catalyst(In_(1)‐Co_(4))(9.7 mmol g_(cat)^(–1) h^(–1))showed five times methanol yields than pure In_(2)O_(3)(2.2 mmol g_(cat)^(–1) h^(–1))(P=4.0 MPa,T=300°C,GHSV=24000 cm^(3)_(STP) g_(cat)^(–1) h^(–1),H_(2):CO_(2)=3).And the cobalt‐catalyzed CO_(2) methanation activity was suppressed,although cobalt was most of the metal *** unravel this selectivity shift,detailed catalysts performance evaluation,together with several in‐situ and ex‐situ characterizations,were employed on cobalt and In‐Co for comparative *** results indicated CO_(2) hydrogenation on cobalt and In‐Co catalyst both followed the formate pathway,and In‐Co reconstructed and generated a surface In_(2)O_(3)‐enriched core‐shell‐like structure under a reductive *** enriched In_(2)O_(3) at the surface significantly enhanced CO_(2) adsorption capacity and well stabilized the intermediates of CO_(2) ***_(2) and carbon‐containing intermediates adsorbed much stronger on In‐Co than cobalt led to a feasible surface C/H ratio,thus allowing the*CH_(3)O to desorb to produce CH_(3)OH instead of being over‐hydrogenated to CH_(4).

摘要：The long atmospheric residence time of CO2 creates an urgent need to add atmospheric carbon drawdown to CO2 regulatory *** and systems biology(SSB),which enables manipulation of cellular phenotypes,offers a powerful approach to amplifying and adding new possibilities to current land management practices aimed at reducing atmospheric *** participants(in attendance:Christina Agapakis,George Annas,Adam Arkin,George Church,Robert Cook-Deegan,Charles DeLisi,Dan Drell,Sheldon Glashow,Steve Hamburg,Henry Jacoby,Henry Kelly,Mark Kon,Todd Kuiken,Mary Lidstrom,Mike MacCracken,June Medford,Jerry Melillo,Ron Milo,Pilar Ossorio,Ari Patrinos,Keith Paustian,Kristala Jones Prather,Kent Redford,David Resnik,John Reilly,Richard ***,Daniel Segre,Susan Solomon,Elizabeth Strychalski,Chris Voigt,Dominic Woolf,Stan Wullschleger,and Xiaohan Yang)identified a range of possibilities by which SSB might help reduce greenhouse gas concentrations and which might also contribute to environmental sustainability and *** include,among other possibilities,engineering plants to convert CO2 produced by respiration into a stable carbonate,designing plants with an increased root-to-shoot ratio,and creating plants with the ability to self-fertilize.A number of serious ecological and societal challenges must,however,be confronted and resolved before any such application can be fully assessed,realized,and deployed.

摘要：设计廉价和高效的双功能催化剂应用于CO_(2)还原和O_(2)还原反应(CO_(2)RR和ORR)是实现碳中和的理想选择.因此,本文研制出铌原子分散固定在氮掺杂有序介孔碳(Nb-N-C)上的双功能CO_(2)RR和ORR催化剂用于锌-空气电池(ZAB)自驱动CO_(2)RR.得益于高铌原子利用率和有序介孔结构,Nb-N-C催化剂展现出高达90%的CO法拉第效率,ORR的半波电位活性为0.84 V,ZAB的峰值功率活性为115.6 mW cm-2.此外,采用两个串联的ZABs单元作为自供能CO_(2)RR系统的电源,能够连续将C O_(2)转化为C O.该自供能系统前10小时的C O平均产率为3.75μmol h-1mg-1cat.理论计算表明,铌原子分散固定在氮掺杂的碳上形成Nb–N配位键,从而有效地降低CO_(2)RR的决速中间体*COOH和ORR的决速中间体*O的生成能垒.

摘要：Anchoring molecular cocatalysts on semiconductors has been recognized as a general strategy to boost the charge separation efficiency required for efficient ***,the effect of molecular cocatalysts on energy funneling(i.e.,directional energy transfer)inside semiconductor photocatalysts has not been demonstrated *** we prepared CdS nanorods with both thin and thick rods and anchored the conjugated molecules 2‐mercaptobenzimidazole(MBI)and cobalt molecular catalysts(MCoA)sequentially onto the surface of *** absorption measurements revealed that MBI molecules facilitated energy funneling from thin to thick rods by the electronic coupling between thin and thick nanorods,which is essentially a light‐harvesting antenna approach to enhance the charge generation efficiency in the reaction center(here the thick rods).Moreover,MBI and MCoA molecules selectively extracted photogenerated holes and electrons of CdS nanorods rapidly,leading to efficient charge ***,CdS/MBI/MCoA displayed 15 times enhanced photocatalytic H_(2) evolution(1.65 mL)than pure CdS(0.11 mL)over 3 h of *** amount of H_(2) evolution reached 60 mL over 48 h of illumination with a high turnover number of 26294 and an apparent quantum efficiency of 71%at 420 *** study demonstrates a novel design principle for next‐generation photocatalysts.