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Jun 09, 2022

Volume 8Issue 6p1537-1788
On the cover: Deng, Zhou, and co-workers (page 1637) report an in situ interface imaging technique to track the evolution of the crystal interface during the growth of a metal-organic framework (MOF) in solution. The authors measured critical kinetic parameters and propose a new mechanism for MOF growth, where the assembly and fragmentation of secondary building units are followed by fragment accumulation in a reversible transition layer at the interface....
On the cover: Deng, Zhou, and co-workers (page 1637) report an in situ interface imaging technique to track the evolution of the crystal interface during the growth of a metal-organic framework (MOF) in solution. The authors measured critical kinetic parameters and propose a new mechanism for MOF growth, where the assembly and fragmentation of secondary building units are followed by fragment accumulation in a reversible transition layer at the interface.
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In This Issue

  • In this issue

    In This Issue highlights the most exciting articles of the current issue with short editorial pieces written by the corresponding handling editors.

Previews

  • Precious-metal-free catalyst could afford cost-effective green hydrogen

    • Laurie A. King,
    • Yagya N. Regmi
    Water splitting is an important technology for green hydrogen production. However, the sluggish kinetics of the anodic oxygen evolution reaction limit device performance. Furthermore, under acidic conditions, sparse and expensive iridium-based catalysts are required. In the May issue of Chem, Lu et al. explored mild electrochemical oxidation treatments to transform graphite flakes into promising oxygen evolution reaction (OER) catalysts.

  • Evolution of MOF single crystals

    • Omar M. Yaghi
    The mechanism of MOF crystal growth is fundamentally important to their design. In this issue of Chem, Deng and co-workers use an optical method to visualize and track the crystal interface during MOF growth. They derive a reaction kinetic equation for individual crystals of MOFs, thereby offering guidance to MOF synthesis.

  • Perrhenate recognition within a superphane cavity

    • Bin Chen,
    • Juan Diwu,
    • Shuao Wang
    In the May issue of Cell Reports Physical Science, Gale and co-workers document a lantern-like receptor (superphane) containing a tailor-made cavity for selective binding of perrhenate anion, leading to an extraordinary capability to separate perrhenate from complex aqueous solutions by either liquid-liquid extraction or solid-phase extraction.

  • In situ generation of active ⋅OH on Co-SrTiO3 tandem catalyst for conversion of methane to methanol

    • Zhongbin Luo,
    • Yung-Kang Peng,
    • Haifeng Xiong
    Recently in Chem Catalysis, He and co-workers proposed the efficient conversion of methane to methanol under moderate conditions via the active O species in situ generated from photo-splitting of H2O over Co-SrTiO3 tandem catalysts. Using characterization techniques, the authors determined the intermediates and mechanism of the reaction.

  • Does in-situ-generated H2O2 promote important industrial reactions?

    • Linfang Lu,
    • Baizeng Fang
    Recently in Science, Hutchings and co-workers reported an efficient TS-1-supported AuPd alloy nanoparticle catalyst that produced cyclohexanone oxime with a selectivity > 95% through the in-situ-generated H2O2, comparable to the current industrial route. The use of in-situ-generated H2O2 can achieve great cost savings in current industrial production of oxime and is believed to have bright prospects in other industrial chemical reactions that need H2O2.

  • Membrane catalysts eliminate trace pollutants

    • Jing Li,
    • Xiao-Yu Yang
    The presence of residues in products generated by high-efficiency catalytic reactions is detrimental. In a recent work published in Nature Nanotechnology by Andrea Schäfer and colleagues, membrane catalysts are shown to promote processes while enhancing water purification by degradation of micropollutants via filtration-driven effective collision.

Perspectives

  • Nanocomposite DNA hydrogels emerging as programmable and bioinstructive materials systems

    • Yong Hu,
    • Chunhai Fan
    The innovation of DNA hydrogels has led to the development of programmable nanocomposite DNA hydrogels that are now emerging as bioinstructive materials systems for fundamental and applied research at the crossroads of chemistry, materials, and biology. Due to the feasible synthesis of various colloidal materials and DNA-colloid conjugates, nanocomposite DNA hydrogels can be rationally designed and assembled with tunable physiochemical property as well as integrated functionalities, thereby responding to external physical cues, exhibiting catalytic activities, or acting as therapeutic agents. Furthermore, the implementation of such tailorable substrata enables grafting, colonization, and control of eukaryotic and prokaryotic cells for cell-substrate engineering. It can be anticipated that the integration of nanocomposite DNA hydrogels with microfluidic systems or DNA surface technology might facilitate the development of modern integrated systems and platforms for widespread applications in materials and life sciences.

  • Challenges for photocatalytic overall water splitting

    • Chuanbiao Bie,
    • Linxi Wang,
    • Jiaguo Yu
    Photocatalytic overall water splitting is theoretically and practically hard to achieve. The unfavorable thermodynamics, sluggish kinetics (especially for the oxygen evolution reaction), dissolved oxygen, and severe backward and side reactions greatly limit its efficiency. Therefore, hydrogen production via photocatalytic overall water splitting is challenging even in the future. Whether photocatalytic overall water splitting is the best option for hydrogen production remains questionable.

Reviews

  • How computations accelerate electrocatalyst discovery

    • Chongyi Ling,
    • Yu Cui,
    • Shuaihua Lu,
    • Xiaowan Bai,
    • Jinlan Wang
    The development of efficient catalysts is the key to the practical application of electrochemical energy conversion, which is regarded as a promising way to alleviate global energy shortage and environmental crisis. In this review, the role of computations in electrocatalyst discovery was introduced and discussed, including the identification of active sites, reaction mechanisms, activity descriptors, and promising electrocatalysts.

  • Membrane design for non-aqueous redox flow batteries: Current status and path forward

    • Michelle L. Lehmann,
    • Landon Tyler,
    • Ethan C. Self,
    • Guang Yang,
    • Jagjit Nanda,
    • Tomonori Saito
    Long-duration energy storage technologies are necessary to enable the widespread adoption of renewable energy sources. Non-aqueous redox flow batteries (NARFBs) represent one of the key technologies in long-duration storage applications due to their flexible material selection and wide operating voltage. Membranes play a vital role in these next-generation energy storage technologies. Here, we survey polymer membranes for NARFBs and reveal factors that influence membrane properties in non-aqueous electrolytes that provide important design principles for developing next-generation membranes for NARFBs.

Articles

  • Determining factors in the growth of MOF single crystals unveiled by in situ interface imaging

    • Jinli Han,
    • Xudong He,
    • Jin Liu,
    • Ruijian Ming,
    • Mohan Lin,
    • Hui Li,
    • Xiaochun Zhou,
    • Hexiang Deng
    Crystal interface evolution is monitored by super-resolution technique during the growth of small MOF crystals into larger ones, in solution. The reaction orders for metal ion and organic linker are determined by isolation method and found to be independent from the corresponding MOF chemical formulas. This leads to the proposal of a new mechanism for MOF growth, involving the assembling and fragmentation of secondary building units, followed by fragment accumulation in a reversible transition layer at the interface of the MOF crystal.

  • Fe binuclear sites convert methane to acetic acid with ultrahigh selectivity

    • Bo Wu,
    • Tiejun Lin,
    • Zhengxing Lu,
    • Xing Yu,
    • Min Huang,
    • Ruoou Yang,
    • Caiqi Wang,
    • Chen Tian,
    • Jiong Li,
    • Yuhan Sun,
    • Liangshu Zhong
    Fe binuclear sites supported on ZSM-5 were prepared and used for the production of CH3COOH with ultrahigh selectivity from CH4 conversion at ambient temperature. The unique structure of [Fe(III)–(μO)2–Fe(III)–(OH)2] not only improved the catalytic activity by enhancing the utilization efficiency of H2O2 but also preferentially promoted the formation of CH3COOH by the direct coupling of ·CH3 with CO∗ and OH∗.

  • Exceptionally active and stable RuO2 with interstitial carbon for water oxidation in acid

    • Juan Wang,
    • Chen Cheng,
    • Qi Yuan,
    • Hao Yang,
    • Fanqi Meng,
    • Qinghua Zhang,
    • Lin Gu,
    • Jianlei Cao,
    • Leigang Li,
    • Shu-Chih Haw,
    • Qi Shao,
    • Liang Zhang,
    • Tao Cheng,
    • Feng Jiao,
    • Xiaoqing Huang
    A robust acidic OER electrocatalyst C-RuO2-RuSe with interstitial carbon was designed and constructed by simultaneous Se evaporation and C combustion of the C-supported amorphous RuSe2. Experimental and theoretical results prove that the interstitial C can elongate the Ru–O bonds to enhance the binding energy for ∗O and thus lead to a significant increase in stability. This project provides a new perspective to improve electrocatalytic OER stability under acidic conditions by inducing interstitial atoms.

  • Metal-organic frameworks enable regio- and stereo-selective functionalization of aldehydes and ketones

    • Yin Zhang,
    • Jun Guo,
    • Jiangwei Zhang,
    • Xueying Qiu,
    • Xiaofei Zhang,
    • Jianyu Han,
    • Binhao Zhang,
    • Chang Long,
    • Yanan Shi,
    • Zhongjie Yang,
    • Wenshi Zhao,
    • Zhiyong Tang
    To satisfy the tremendous demand for chiral molecules, recyclable and efficient catalysts are always desired. In this report, three types of asymmetric reactions have been implemented with tunable metal-organic frameworks as catalysts for transformations of abundant aldehydes and ketones. The superior tunability of catalysts relies on the switchable feature of their structure and composition, which are confirmed by both experiments and theoretical calculations.

  • TADF molecules with π-extended acceptors for simplified high-efficiency blue and white organic light-emitting diodes

    • Xiangchen Hong,
    • Dongdong Zhang,
    • Chen Yin,
    • Qi Wang,
    • Yuewei Zhang,
    • Tianyu Huang,
    • Jinbei Wei,
    • Xuan Zeng,
    • Guoyun Meng,
    • Xiang Wang,
    • Guomeng Li,
    • Dezhi Yang,
    • Dongge Ma,
    • Lian Duan
    By elegantly extending the acceptor π-system, we have successfully developed highly efficient and stable blue thermally activated delayed fluorescence (TADF) emitters based on carbazole-benzonitrile derivatives with preferred horizontal orientation. Both blue and white organic light-emitting diodes based on them achieve impressive efficiencies and high stabilities, making a promising step toward the practical applications of blue TADF emitters.

  • Spin-enabled photochemistry using nanocrystal-molecule hybrids

    • Meng Liu,
    • Junhui Wang,
    • Guijie Liang,
    • Xiao Luo,
    • Guohui Zhao,
    • Shan He,
    • Lifeng Wang,
    • Wenfei Liang,
    • Juntao Li,
    • Kaifeng Wu
    The short spin lifetimes of CsPbBr3 perovskite nanocrystals can find immediate applications in molecular photochemistry that largely relies on spin-relaxed triplet excited states. In CsPbBr3 nanocrystals surface-anchored with rhodamine B molecules, excitation of either the nanocrystal or the molecule induces charge separation, and a rapid spin-flip of the carrier inside the nanocrystal enables high-yield formation of molecular triplets through charge recombination. Leveraging the complementary spectral coverage of CsPbBr3 and rhodamine, we achieve efficient white-light-driven triplet-fusion photon upconversion and singlet-oxygen generation.

  • Unified sensing of the concentration and enantiomeric composition of chiral compounds with an achiral probe

    • Archita Sripada,
    • F. Yushra Thanzeel,
    • Christian Wolf
    A unified CD sensing strategy that achieves simultaneous determination of the enantiomeric composition and the concentration or reaction yield of chiral compounds is described. This important task is achieved by using a readily available achiral probe in a straightforward organic-reaction-based assay that was tested with chiral amines, amino alcohols, and amino acids. Unified CD sensing can be easily adapted, offers significant speed, labor, and cost benefits over traditional techniques at reduced chemical waste production, and is universally applicable.

  • A homogeneous high-throughput array for the detection and discrimination of influenza A viruses

    • Wei-Tao Dou,
    • Xiang Wang,
    • Tingting Liu,
    • Suwen Zhao,
    • Jiao-Jiao Liu,
    • Yao Yan,
    • Jun Li,
    • Chi-Yu Zhang,
    • Adam C. Sedgwick,
    • He Tian,
    • Jonathan L. Sessler,
    • Dong-Ming Zhou,
    • Xiao-Peng He
    We report a high-throughput “glycoVIEgen” array for the simultaneous detection and determination of the host specificity of influenza A viruses (IAVs). Our array system enables the detection of IAVs with discrimination against other viral species and the determination of IAVs specific to individual species. Moreover, our glycoVIEgen array can classify the level of IAV mutations isolated from infected human individuals. Finally, this approach is amenable to performing quality control on developed IAV vaccines and confirming matched hemagglutinin specificities between vaccines and IAV strains.

  • Catalytic reductive ring opening of epoxides enabled by zirconocene and photoredox catalysis

    • Kazuhiro Aida,
    • Marina Hirao,
    • Aiko Funabashi,
    • Natsuhiko Sugimura,
    • Eisuke Ota,
    • Junichiro Yamaguchi
    Open Access
    The reductive ring opening of epoxides serves as an effective tool for chemists to enable access to a broad array of alcohols from readily available epoxides via a radical pathway. Titanocene has been exclusively employed for the transformation over the last 30 years. Herein, we report an unprecedented zirconocene-catalyzed ring opening of epoxide enabled by visible-light catalysis. The mild and catalytic protocol exhibited broad functional group tolerance. We believe that this method provides a new perspective on zirconocene-mediated photocatalysis.

  • Computationally designed ligands enable tunable borylation of remote C–H bonds in arenes

    • Wenju Chang,
    • Yu Chen,
    • Shuo Lu,
    • Hongyun Jiao,
    • Yajun Wang,
    • Tianyu Zheng,
    • Zhuangzhi Shi,
    • Yingbin Han,
    • Yi Lu,
    • Yi Wang,
    • Yi Pan,
    • Jin-Quan Yu,
    • Kendall N. Houk,
    • Fang Liu,
    • Yong Liang
    Remote selective C–H functionalization of arenes is challenging because meta- and para-C–H bonds are far away from the directing group but are adjacent with small differences in reactivity. Here, guided by DFT calculations, we designed two sets of ligands to accomplish the meta- and para-selective borylation of arenes. Various hydrogen bond acceptors can be used as multi-transformable directing groups. The tunable site selectivity and rich transformations of both directing groups and formed C–B bonds increase the diversity of multi-substituted arenes dramatically.
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