Alkaline CO2 electrolysis can produce multicarbon (C2+) products such as ethylene and acetate, yet suffers from low CO2 utilization efficiency.Ttandem electrolysis, which connects solid oxide or acidic CO2 electrolysis to CO and alkaline CO electrolysis to C2+ products in sequential electrolyzers, is a carbon-efficient route. However, to date, CO electrolysis generally shows high current density and selectivity for C2+ products, but selective generation of a specific C2+ product is still challenging.Recently, a research team led by Profs. WANG Guoxiong and GAO Dunfeng from the Dalian Institute of Chemical Physics (DICP) of the Chinese Academy of Sciences (CAS) has proposed a new strategy by constructing metal-organic interfaces for CO electrolysis to acetate with high selectivity.This study was published in Angewandte Chemie International Edition on Sep. 25.Boosting CO electrolysis to acetate with Cu-organic interface (Image by RONG Youwen)The researchers tuned the reaction microenvironments surrounding catalytically active sites by constructing Cu-organic interfaces through in-situ electrochemical reconstruction of molecular Cu complexes. Benefiting from the favorable reaction microenvironment, they achieved good catalytic performance for CO electrolysis to acetate, in terms of current density, Faradaic efficiency, and yield.With a copper phthalocyanine (CuPc) electrode measured in a home-made alkaline membrane electrode assembly (MEA) electrolyzer, they obtained an acetate Faradaic efficiency as high as 84.2% and an acetate carbon selectivity of 92.1% at 500 mA cm-2. The maximum acetate partial current density and formation rate reached 605 mA cm-2 and 0.38 mmol min-1, respectively, translating into an acetate yield as high as 63.4%.The Cu-organic interface created a favorable reaction microenvironment that enhanced *CO adsorption, lowered the energy barrier for C-C coupling, and facilitated the formation of CH3COOH over other multicarbon products, thus rationalizing the selective acetate production."Our study highlights the potential of constructing metal-organic interfaces for tailoring reaction microenvironments for highly selective production of a specific C2+ product from CO electrolysis," said Prof. GAO.The above work was supported by the National Key R&D Program of China, the National Natural Science Foundation of China, the Collaborative Innovation Center of Chemistry for Energy Materials, and the Youth Innovation Fund of DICP.

　　Acetylene hydrogenation to ethylene (AHE) in combination with acetylene production from coal pyrolysis is considered as a promising alternative to the traditional petroleum-based ethylene production route. However, thermocatalytic AHE (T-AHE) process often suffers from high temperatures (100-300 oC) and high consumption of molecular hydrogen (H2).
　　Recently, a research group led by Prof. DENG Dehui and Assoc. Prof. YU Liang from the Dalian Institute of Chemical Physics (DICP) of the Chinese Academy of Sciences (CAS) realized a new process of acetylene hydrogenation to ethylene by directly using water as hydrogen source (WAHE) and low-cost CO as oxygen acceptor over a Au/α-MoC catalyst.
　　This study was published in Nature Catalysis on September 28.
　　Acetylene hydrogenation to ethylene by water at low temperature on a Au/α-MoC catalyst (Image by HUANG Rui)
　　The hydrogenation of acetylene can proceed by a H2-based thermocatalytic route or H2O-based electrocatalytic route. The thermocatalytic AHE is energy
　　demanding due to the requirement of relatively high temperature and H2 consumption, since H2 is also industrially produced by energy-intensive processes such as steam methane reforming (SMR) and water gas shift (WGS) reaction.
　　The electrochemical AHE (E-AHE) process is advantageous as it directly uses electrochemically-generated active hydrogen species from water to hydrogenate acetylene without involving the unnecessary formation of H2. 
　　The WAHE process delivered over 99% acetylene conversion and high ethylene selectivity of 83% at 80 oC.
　　Mechanistic studies revealed that in-situ generated hydroxyl species from water dissociation at the boundary of Au and α-MoC, serving as mild reductants, enabled the selective semi-hydrogenation reaction with residual O removed by CO. This process circumvents H2 consumption in the classical route and opens avenues for energy-efficient acetylene hydrogenation by water at low temperature.
　　This work was supported by the National Key R&D Program of China, the National Natural Science Foundation of China and the Strategic Priority Research Program of CAS.

　　A research group led by Prof. DENG Dehui from the Dalian Institute of Chemical Physics (DICP) of the Chinese Academy of Sciences (CAS) has realized direct conversion of air to nitric acid (HNO3) under ambient conditions through a hydroxyl radical (·OH)-mediated hetero-homogeneous electro-chemical route.
　　In the route, the N2 was oxidized to HNO3 by employing heterogeneous electroreduction of O2 to H2O2 on a graphite rod catalyst combined with homogeneous Fe2+-induced dissociation of the in situ generated H2O2 to OH· as reactive oxidation species.
　　The study was published in Nature Synthesis on September 25.
　　HNO3, as an important chemical building block, is produced industrially from the oxidation of ammonia via the Ostwald process, which requires high temperatures above 800 oC. In this process, the feed ammonia gas is industrially synthesized via the energy-intensive Haber-Bosch method typically operating at high temperatures (400 to 500 oC) and pressures (20 to 50 MPa).
　　Direct conversion of dinitrogen (N2) and oxygen (O2) in the air to HNO3 under mild conditions is a promising and sustainable route for the production of HNO3. However, the thermodynamic and kinetic restrictions of this reaction as well as the high stability of N2 and the low activity of O2, make it a challenge to achieve co-activation and efficient conversion of the two molecules in the air toward HNO3 synthesis.
　　Schematic illustration for the hetero-homogeneous electrochemical conversion of air to HNO3 (Image by CHEN Shiming and YU Liang)
　　In this study, the researchers developed a hetero-homogeneous electro-chemical route for the direct conversion of air to HNO3 at the cathode compartment. At the cathodic potential of 0 V vs. RHE, the faradaic efficiency of nitric acid was as high as 25.37%, and the selectivity was over 99%, which was superior than the previously reported electrocatalytic oxidation of N2 at the anode with high potentials above 1.23 V vs. RHE.
　　Multiple in situ spectroscopic characterizations and theoretical calculations revealed that ·OH produced from Fe2+-induced dissociation of in-situ generated H2O2 could efficiently activate N2. This delivered a high HNO3 productivity of 141.83 μmol·h-1·gFe-1 which was 225 times that of directly using H2O2 as the oxidant.
　　"This process for HNO3 synthesis from N2 and O2 effectively avoids the traditional high-temperature and high-pressure reaction conditions, and provides a new route for the co-activation and efficient conversion of N2 and O2 under mild conditions," said Prof. DENG.
　　The above work was supported by the National Natural Science Foundation of China, the National Key R&D Program of China, and the Strategic Priority Research Program of CAS.

Direct conversion of methane (CH4) to high value-added chemicals at room temperature, by directly using abundant and low-cost molecular oxygen (O2) as an oxidant, is an ideal route for CH4 utilization. But it remains a challenge owing to the chemical inertness of methane and low activity of O2.Recently, a research group led by Prof. DENG Dehui and Assoc. Prof. YU Liang from the Dalian Institute of Chemical Physics (DICP) of the Chinese Academy of Sciences (CAS) realized direct CH4 conversion to C1 oxygenates (CH3OH, HOCH2OH and HCOOH) with O2 at room temperature (25 oC) over an edge-rich MoS2 catalyst.This study was published in Nature Catalysis on September 21.Room-temperature CH4 conversion by O2 over bi-Mo sites confined in MoS2 edge (Image by MAO Jun and LIU Huan)Catalytic conversion of methane to high value-added chemicals is a tough problem due to the low polarization rate and high C-H bond energy (439 kJ mol-1) of methane.Typical catalytic conversion of CH4 usually operates at high temperatures (over 600 oC), or in the aid of strong oxidants (such as fuming sulfuric acid) or external fields (such as plasma). Nevertheless, such harsh reaction easily leads to excessive conversion of the target product, such as overoxidation to CO2.Direct conversion of CH4 and O2 at low temperatures or even at room temperature is an appealing strategy for CH4 conversion. However, it is challenging due to the difficulty in continuous formation of active oxygen species under mild conditions for C-H activation.In situ characterizations and theoretical calculations demonstrated that the unique binuclear molybdenum (bi-Mo) site of sulfur vacancies at the MoS2 edge was able to directly dissociate O2 to form O=Mo=O* active species at 25 oC, which could activate the C-H bond of CH4 and thereby driving the catalytic conversion of CH4 to C1 oxygenates via CH3O* intermediates at room temperature.In this study, the researchers achieved CH4 conversion of up to 4.2% with a high selectivity of over 99% for the C1 oxygenates for CH4 conversion by O2 at room temperature.This work was supported by the National Key R&D Program of China, the National Natural Science Foundation of China and the Strategic Priority Research Program of CAS.

　　Hydrogenation of carbon dioxide (CO2) to formate, an important chemical widely used in leather, textile, mining industry, etc., is an attractive atom-economic route for the utilization of this greenhouse gas.
　　Non-precious metal-based catalysts for the CO2 hydrogenation to formate suffered from either low activity or low stability. It's still a challenge to develop low-cost and high-performance catalysts for CO2 hydrogenation to formate.
　　Recently, a research group led by Prof. DENG Dehui from the Dalian Institute of Chemical Physics (DICP) of the Chinese Academy of Sciences (CAS) developed an edge-rich molybdenum disulfide (ER-MoS2) catalyst for CO2 hydrogenation to formate with superior activity and high stability.
　　The study was published in Angew. Chem. Int. Ed. on July 20 and was selected as hot paper and inside back cover.
　　ER-MoS2 as catalyst for the hydrogenation of CO2 to formate (Image by WANG Zifeng and YU Liang)
　　In this study, the ER-MoS2 with abundant edges delivered a high TOF of 780.7 h-1 with formate selectivity of over 99% at 200 °C, and exhibited a good stability.
　　Multiple experimental characterizations combined with theoretical calculations revealed that sulfur vacancies at MoS2 edges were the active sites and the selective production of formate was enabled via a new water-mediated hydrogenation mechanism, in which surface OH* and H* species from H2O dissociation on the edge-sulfur vacancies served as moderate hydrogenating agents with residual O* reduced by H2.
　　"This work opens new avenue for developing low-cost non-noble metal catalysts for the hydrogenation of CO2 to formate and the revealed water-mediated reaction mechanism also provides insights for designing MoS2-based catalysts for selective hydrogenation reactions," said Prof. DENG.
　　This work was supported by the National Key R&D Program of China, the National Natural Science Foundation of China, the Strategic Priority Research Program of CAS, the LiaoNing Revitalization Talents Program, and Collaborative Innovation Center of Chemistry for Energy Materials (2011. iChEM).

　　Aqueous rechargeable zinc ion batteries are promising in electric grid storage due to their low cost and intrinsic safety. However, the practical implementation is hindered by the poor reversibility of the zinc anode, primarily caused by the chaotic Zn deposition present as dendrite and side reactions.
　　Recently, a research group led by Prof. YANG Weishen and Dr. ZHU Kaiyue from the Dalian Institute of Chemical Physics (DICP) of the Chinese Academy of Sciences (CAS) has proposed a strategy of "ino carriers" by importing macromolecular Zn2+ carriers with a large mass-to-charge ratio to decouple the ion flux from the inhomogeneous electric field and substrate. This strategy provided an efficient pathway to overcome the dendrite and side reaction problems.
　　This study was published in Energy Environmental Science on August 18.
　　By harnessing dynamic MOF nanosheets, zinc anodes underwent a remarkable self-optimization process, resulting in the creation of a highly desirable surface with an unprecedented (002) orientation that is entirely free from any undesirable byproducts (Image by ZHU Kaiyue)
　　The researchers found that metal organic framework (MOF) nanosheets featuring migration capability under an electric field due to their one-dimensional (1D) channel structure and preferential Zn2+ adsorption, as well as unique reductive chemistry due to the weak coordination between ligands and zinc ions, enabling them to serve as dynamic Zn2+ ion carriers.
　　The dynamic MOF nanosheets could continually optimize zinc anode during cycling. Specifically, the zinc electrode was gradually reconstructed towards a horizontally aligned lamellae-like morphology and enhanced (002) texture, showing a relative texture coefficient of a 96.9 (maximum value of 100). This optimization on the morphology and texture could be attributed to the horizontal alignment of Zn2+ ions by the constraints of the MOF nanosheets.
　　Additionally, the presence of MOF ligands contributed to the elimination of undesirable Zn4SO4(OH)6·4H2O byproducts. These byproducts were spontaneously converted into useful MOF nanosheets through unique properties of ligands. Consequently, Zn||Zn symmetric cells and Zn||(NH4)2V10O25·8H2O full cells employing MOF nanosheets in electrolytes exhibited outstanding cycling performance at both low and high rates.
　　"The versatility of the 'ion carrier' holds promise for potential expansion into achieving highly reversible cycling in other rechargeable metal cells, owing to its broad applicability to various ligands, substrates and electrolytes," said Prof. YANG.
　　This work was supported by the National Natural Science Foundation of China and the Youth Innovation Fund of DICP.