{"status":"ok","message-type":"work","message-version":"1.0.0","message":{"indexed":{"date-parts":[[2026,8,12]],"date-time":"2026-08-12T08:36:37Z","timestamp":1786523797916,"version":"build-2736575974"},"reference-count":51,"publisher":"American Chemical Society (ACS)","issue":"31","license":[{"start":{"date-parts":[[2026,7,29]],"date-time":"2026-07-29T00:00:00Z","timestamp":1785283200000},"content-version":"stm-asf","delay-in-days":0,"URL":"https:\/\/doi.org\/10.15223\/policy-029"},{"start":{"date-parts":[[2026,7,29]],"date-time":"2026-07-29T00:00:00Z","timestamp":1785283200000},"content-version":"stm-asf","delay-in-days":0,"URL":"https:\/\/doi.org\/10.15223\/policy-037"},{"start":{"date-parts":[[2026,7,29]],"date-time":"2026-07-29T00:00:00Z","timestamp":1785283200000},"content-version":"stm-asf","delay-in-days":0,"URL":"https:\/\/doi.org\/10.15223\/policy-045"}],"funder":[{"DOI":"10.13039\/501100001809","name":"National Natural Science Foundation of China","doi-asserted-by":"publisher","award":["22406197"],"award-info":[{"award-number":["22406197"]}],"id":[{"id":"10.13039\/501100001809","id-type":"DOI","asserted-by":"publisher"}]},{"name":"ANRF-CRG","award":["CRG\/2023\/000637"],"award-info":[{"award-number":["CRG\/2023\/000637"]}]},{"name":"DST-ASEAN-AISTDF India Collaborative research project","award":["CRD\/2022\/000533"],"award-info":[{"award-number":["CRD\/2022\/000533"]}]},{"name":"CSIR-Indian Institute of Chemical Biology (IICB), Kolkata, India","award":["MLP-002620"],"award-info":[{"award-number":["MLP-002620"]}]},{"name":"CSIR-Indian Institute of Chemical Biology (IICB), Kolkata, India","award":["MMP-075204, HCP-002502"],"award-info":[{"award-number":["MMP-075204, HCP-002502"]}]}],"content-domain":{"domain":[],"crossmark-restriction":false},"short-container-title":[],"published-print":{"date-parts":[[2026,8,12]]},"abstract":"<jats:title>Abstract<\/jats:title>\n                  <jats:p>Achieving high selectivity in alkyne semi-hydrogenation without relying on toxic modifiers remains a major challenge in heterogeneous catalysis. In this work, we have explored the design of a series of heteroatom-functionalized porous organic polymer (POP)-supported Pd catalysts (S-Pd-POP, O-Pd-POP, and N-Pd-POP) to systematically tune catalytic behavior for semi-hydrogenation of 2-methyl-3-butyn-2-ol (MBY) through p-d orbital hybridization. These materials were synthesized via a scalable free-radical polymerization approach followed by Pd incorporation, yielding an amorphous porous network with a distinct electronic microenvironment. Notably, S-Pd-POP contains ultrasmall and well-dispersed Pd nanoparticles (\u223c2.5 nm), significantly smaller than those in O-Pd-POP (\u223c6.5 nm) and N-Pd-POP (\u223c8.5 nm), leading to greater exposure of active sites. Synchrotron X-ray absorption fine structure (XAFS) analysis confirms Pd exists predominantly in a metallic state, while EXAFS results reveal a clear decrease in Pd-Pd coordination numbers from O-Pd-POP to N-Pd-POP to S-Pd-POP, consistent with progressively smaller Pd clusters. We have achieved a good catalytic activity with S-Pd-POP with 95.3% conversion and 97.2% selectivity under mild conditions (60 \u00b0C, 5 bar H2), along with a lower activation energy (24.6 kcal mol-1) than its counterparts. Comprehensive density functional theory calculations validate experimental findings, which show strong overlap between S(p) and Pd(d) orbitals near the Fermi level, indicating pronounced p-d orbital hybridization, which is further supported by significant sulfur-to-Pd electron interaction donation from natural bond orbital analysis. In contrast, nitrogen- and oxygen-based systems show much weaker electronic interactions, corroborating their hydrogenation activity data. In situ ATR-IR spectroscopy studies reveal that the reaction proceeds via weakly bound \u03c0-intermediates, which promote rapid product desorption and effectively suppress over-hydrogenation. Overall, this work highlights p-d orbital hybridization as a key factor governing catalytic selectivity and provides a practical strategy for designing efficient, modifier-free hydrogenation catalysts.<\/jats:p>","DOI":"10.1021\/acsami.6c09011","type":"journal-article","created":{"date-parts":[[2026,8,4]],"date-time":"2026-08-04T13:19:04Z","timestamp":1785849544000},"page":"42582-42598","source":"Crossref","is-referenced-by-count":0,"title":["Porous Organic Microenvironment Unlocks p-d Orbital Hybridization to Enable Precise Semi-Hydrogenation of Alkynol: Bridging Experiment and Computational Insights"],"prefix":"10.1021","volume":"18","author":[{"ORCID":"https:\/\/orcid.org\/0009-0004-6054-4779","authenticated-orcid":true,"given":"Dhruba Jyoti","family":"Deka","sequence":"first","affiliation":[{"name":"CSIR-Indian Institute of Chemical Biology , , 4-Raja S. C. Mullick Road, Jadavpur , ,","place":["Kolkatta, India, 700032"]},{"name":"Academy of Scientific and Innovative Research (AcSIR) , ,","place":["Ghaziabad, India, 201002"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jang Mee","family":"Lee","sequence":"additional","affiliation":[{"name":"RMIT University , , GPO Box 2476 , , ,","place":["Melbourne, VIC, Australia, 3001"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-4313-9331","authenticated-orcid":true,"given":"Bishal","family":"Boro","sequence":"additional","affiliation":[{"name":"CSIR-Indian Institute of Chemical Biology , , 4-Raja S. C. Mullick Road, Jadavpur , ,","place":["Kolkatta, India, 700032"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Tayebeh","family":"Hosseinnejad","sequence":"additional","affiliation":[{"name":"RMIT University , , GPO Box 2476 , , ,","place":["Melbourne, VIC, Australia, 3001"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-7718-7430","authenticated-orcid":true,"given":"Xianwei","family":"Wang","sequence":"additional","affiliation":[{"name":"Chinese Academy of Sciences , , ,","place":["Beijing, China, 100085"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-0896-5168","authenticated-orcid":true,"given":"Duy Quang","family":"Dao","sequence":"additional","affiliation":[{"name":"Duy Tan University , , ,","place":["Da Nang, Vietnam, 550000"]},{"name":"Duy Tan University , , ,","place":["Da Nang, Vietnam, 550000"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-3127-8166","authenticated-orcid":true,"given":"Suresh K.","family":"Bhargava","sequence":"additional","affiliation":[{"name":"RMIT University , , GPO Box 2476 , , ,","place":["Melbourne, VIC, Australia, 3001"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Paramita","family":"Koley","sequence":"additional","affiliation":[{"name":"RMIT University , , GPO Box 2476 , , ,","place":["Melbourne, VIC, Australia, 3001"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-7813-2108","authenticated-orcid":true,"given":"John","family":"Mondal","sequence":"additional","affiliation":[{"name":"CSIR-Indian Institute of Chemical Biology , , 4-Raja S. 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